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Measurements of The Distribution and Behaviour of Beryllium-7 in The Natural Environment
Measurements of The Distribution and Behaviour of Beryllium-7 in The Natural Environment
ENVIRONMENT
Che Doering
Doctor of Philosophy
2007
i
KEYWORDS
rays, atmosphere, deposition, soil, surface air, atmospheric transport, erosion, depositional
ii
ABSTRACT
carried in the atmosphere attached to aerosols and is deposited on land and ocean surfaces
by wet and dry deposition processes. Beryllium-7 decays by electron capture to lithium-7
foundation for the development of nuclear techniques for the evaluation of environmental
problems.
iii
LIST OF PUBLICATIONS
210
Doering, C., Akber, R., Heijnis, H., 2006. Vertical distributions of Pb excess, 7Be and
137
Cs in selected grass covered soils in Southeast Queensland, Australia. Journal of
Doering, C., Akber, R., submitted. Beryllium-7 in near-surface air and deposition at
Doering, C., Akber, R., submitted. Describing the annual cyclic behaviour of 7Be
iv
TABLE OF CONTENTS
CHAPTER ONE 1
INTRODUCTION
CHAPTER TWO 4
LITERATURE REVIEW
2.1 Introduction 4
2.9 Deposition 15
References 29
CHAPTER THREE 43
210
VERTICAL DISTRIBUTIONS OF Pb EXCESS, 7Be AND 137
Cs IN SELECTED
v
3.1 Introduction 46
3.2.2 Soils 47
3.3 Results 52
210
3.3.1 Pbex and 7Be areal activity densities 52
fluxes 56
erosion studies 62
3.4 Conclusions 64
References 65
CHAPTER FOUR 68
AUSTRALIA
4.1 Introduction 71
4.4 Conclusion 80
References 81
vi
CHAPTER FIVE 83
5.1 Introduction 86
References 101
CONCLUDING REMARKS
vii
LIST OF TABLES
Table 2.1. Average surface air concentrations of 7Be at different locations. Data is
Table 2.2. Annual 7Be deposition and rainfall at different locations. Data is sorted in
Table 2.3. Total 7Be areal activity densities at undisturbed sites. Data is sorted in
Table 3.1. Site location, annual rainfall rate, and physical and chemical properties of
the soils (moisture content, composition and particle size distribution are
Table 3.2. Accumulated 210Pbex, 7Be and 137Cs areal activity density in the surface 10
Table 4.2. Summary of 7Be deposition measurements at Brisbane during the years
Table 4.3. Comparison of measured and calculated net cumulative 7Be areal activity
88–89)
Table 5.3. Values of linear correlation coefficient (R) and Spearman correlation
viii
LIST OF FIGURES
Figure 3.1. Location of the sampling sites and map of Australia (inset). (p. 48)
210
Figure 3.2. Pbex (top) and 7Be (bottom) cumulative areal activity density profiles
indicates the line of equality. Errors in 226Ra, 210Pb and 238U are typically
cm depth. The site key is the same as that shown in Figure 3.2. The solid
line represents the best fitting linear function to the data. The dotted lines
Figure 4.1. Percent deviation of monthly average 7Be concentrations from the annual
Figure 4.2. Monthly 7Be deposition (columns) and rainfall (solid circles) at Brisbane
Figure 4.3. Monthly 7Be deposition (Y) plotted against monthly rainfall (X). The
solid line represents the linear least squares regression line. (p. 77)
Figure 4.4. Calculated net cumulative 7Be areal activity density (columns) and
ix
The solid line is the decay curve for 7Be activity deposited before January
2000. The dashed line shows the trend in rainfall. (p. 79)
Figure 5.1. Map of Oceania showing location of 7Be measurement stations. (p. 87)
Figure 5.3. Latitude-time isopleth diagram of the zonal averaged ratio of the mean of
90
monthly Sr concentrations in surface air. From Rehfeld and Heimann
Figure 5.4. Mean of monthly 7Be deviations (filled circles) at American Samoa (top
panel), Brisbane (middle panel) and Cape Grim (bottom panel), and mean
of monthly 90Sr deviations (open circles) at the equivalent latitude. (p. 98)
x
STATEMENT OF ORIGINAL AUTHORSHIP
The work contained in this thesis has not been previously submitted for a degree or diploma
at any other tertiary education institution. To the best of my knowledge and belief, the
thesis contains no material previously published or written by another person except where
Signed: ……………………………..
Date: ……………………………..
xi
CHAPTER ONE
INTRODUCTION
general categories: (1) primordial radionuclides, i.e., nuclides which have survived since
the time when the elements formed, and their progeny nuclides; (2) cosmogenic
nuclear weapons. Radioecology is the study of the occurrence of these radionuclides in the
natural environment. This includes the atmosphere, hydrosphere and lithosphere. Studies of
the timescales over which natural systems are changing or evolving and the underlying
mechanistic causes. They can also be used to assess the radiological or radioecological
cosmic-ray-produced neutrons and protons disintegrate the atomic nucleus of nitrogen and
oxygen into lighter fragments. It has a relatively short half-life of approximately 53 days.
7
Be is found naturally in air, rainwater, soils and sediments, vegetation, as well as lake,
estuarine and ocean waters. The use of 7Be as a tracer of natural processes has recently been
realised, and a number of nuclear techniques have been developed to support ongoing
7
research in this area. Nevertheless, most applications of Be require a detailed
still incomplete. Therefore, studies of 7Be, such as those presented in this thesis, will
greatly add to our understanding of the behaviour of this radionuclide in the environment
1
1.2 Research objectives
The overall objectives of this research were to (1) investigate the distribution of
7
Be in soils within Southeast Queensland in order to evaluate the potential use of this
radionuclide as a tracer of soil erosion; and (2) investigate the atmospheric cycle of 7Be
within the troposphere, both in Southeast Queensland and the Oceania region. These
research objectives were met through a number of subsidiary aims, which were to (1)
measure 7Be activity in soils and grasses and identify factors controlling the areal activity
density of this radionuclide; (2) measure 7Be activity in wet and dry deposition and identify
factors controlling the depositional flux of this radionuclide; (3) measure 7Be activity in
surface air; and (4) describe the annual cycle of 7Be concentrations in surface air and
purpose of this review is to examine the current state of knowledge surrounding 7Be. It
covers aspects of 7Be nuclear properties, activity measurement, production, distribution and
behaviour in natural systems, as well as applications for tracing natural processes. This
chapter provides a foundation of understanding for the results and discussions presented in
Queensland are presented in Chapter Three as a published paper. These are the first such
measurements to be reported for the region. It is recognised that soil erosion is a major
factor contributing to land degradation in Southeast Queensland. This is due in part to high
rates of population growth and urban development. Nuclear techniques can be used to
assess rates of short- and medium-term soil erosion. However, of critical importance to
2
such assessments is knowledge of the distribution of radionuclides within the soil profile
and factors that affect their areal activity density. In addition to 7Be, distributions of
naturally occurring lead-210 excess (210Pbex) and the artificial radionuclide caesium-137
submitted paper. Such measurements are fundamentally important for understanding factors
that deliver 7Be to terrestrial systems and affect its areal activity density in soils and
overlying vegetation. The measurements presented in this chapter were performed over
three complete years so that any seasonal or annual changes in the depositional flux of this
radionuclide could be observed. The study compares values of 7Be areal activity density
calculated from measured depositional fluxes with those measured directly in soils and
grasses. It identifies seasonality in rainfall and the 7Be half-life itself to be important factors
controlling the areal activity density of 7Be in Southeast Queensland. This chapter also
presents measurements of 7Be in surface air and investigates the relationship between 7Be
A study of the annual cycle of 7Be concentrations in surface air in the Oceania
region is presented in Chapter Five as a submitted paper. The annual cycle is a defining
feature of this radionuclide in surface air and is thought to be the product of a number of
meteorological factors. This study analyses data collected throughout the Oceania region
over the past years and shows that the observed annual cycle can be described by a
sinusoidal model. In addition, by comparison with available artificial radionuclide data for
transport of air within the troposphere to be active atmospheric processes controlling the
3
CHAPTER TWO
LITERATURE REVIEW*
*The literature survey for this review was finalised on January 31, 2007.
2.1 Introduction
result of neutron and proton induced reactions with nitrogen and oxygen nuclei. It was first
measured by Arnold and Al-Salih (1955) in rainwater samples collected at Chicago IL and
Lafayette IN (United States) between 1953 and 1954. Cruikshank et al. (1956) soon after
reported on the presence of this radionuclide attached to aerosols in surface air. Since these
pioneering efforts, numerous papers have been written on the production, concentration,
distribution and application of 7Be in the environment. This review summarises the main
findings of a large number of these contributions and examines the current state of
decay by this mechanism. The presently adopted half-life for the transmutation 7Be + e- Æ
7
Li + ν is 53.22 ± 0.06 days (Tilley et al., 2002). The decay of 7Be can proceed either
directly to the 7Li ground state or to the first excited state in 7Li. The branching ratio to the
first excited state is 10.44 ± 0.04 % (Tilley et al., 2002). This decay then proceeds to the 7Li
ground state by prompt gamma-ray emission with energy of approximately 477.6 keV. 7Be
cannot transmute to 7Li by positron (β+) decay as this transition can be shown to be
4
2.3 Activity measurement
7
Be activity is measured through gamma spectrometry. Early investigators utilised
sodium iodide (NaI) detectors for analysis of precipitation and air samples. However, the
relatively low resolution of these detectors and the presence of certain artificial
radionuclides in the environment due to atmospheric nuclear weapon tests (e.g. antimony-
125, ruthenium-103 and rhodium-106) meant that the characteristic 477.6 keV peak from
the decay of 7Be could not be distinguished. Chemical separations were required for
iron hydroxides and other hydroxide phases (see, e.g., Arnold and Al-Salih, 1955;
Cruikshank et al., 1956; Goel et al., 1959). In recent decades germanium detectors have
been widely used for measurement of 7Be activity. These detectors have much higher
energy resolution than their NaI counterparts and in most instances environmental samples
protons disintegrate the atomic nucleus of atmospheric nitrogen and oxygen into lighter
global in extent, and depends upon the flux of cosmic-ray-produced neutrons and protons
traversing the atmosphere, the density of target nitrogen and oxygen nuclei, and an energy
dependent production cross-section (Lal et al., 1958; Lal and Peters, 1962; Lal and Peters,
1967; Nagai et al., 2000). Its main production site is in the stratosphere (approx. 70 %),
though it is also produced in some abundance within the troposphere (approx. 30 %). Lal
and Peters (1962, 1967) calculated 7Be production rates in the atmosphere from available
reactions involving nitrogen and oxygen and reported a global average value of 810 atoms
m-2 s-1. This value has been adopted by the United Nations Scientific Committee on the
5
Effects of Atomic Radiation (UNSCEAR) for the purpose of reporting 7Be production rates
in the atmosphere (UNSCEAR, 2000). Average production rates of 7Be in the atmosphere
have also been determined by several other investigators through a variety of methods and
values ranging from around 100 to 1100 atoms m-2 s-1 are reported in the literature (Arnold
and Al-Salih, 1955; Benioff, 1956; Cruikshank et al., 1956; Lal et al., 1958; Lal et al.,
1960a; Masarik and Reedy, 1995; Masarik and Beer, 1999; Nagai et al., 2000; O’Brien,
The work of Lal and Peters (1962, 1967) shows that 7Be production rates in the
atmosphere vary with latitude and altitude. For all levels of the atmosphere production rates
increase with increasing latitude. For all latitudes the rate of production decreases by
around two orders of magnitude between the lower stratosphere and the surface air. These
authors also report 7Be production rates to vary with the 11 year sunspot cycle. Lower rates
of production are expected at solar maximum due to a decrease in the galactic cosmic-ray
flux to Earth and vice-versa. Masarik and Beer (1999) used a computer model to investigate
geomagnetic field intensity. They found that for radionuclides formed through spallation
reactions the production rate at solar minimum was around 1.15 times higher compared to
the average over a complete solar cycle, and the rates at solar maximum were about 0.85
times the average rates. There is also evidence to suggest that solar energetic particle events
may temporarily perturb 7Be production rates and concentrations in the atmosphere
(Masarik and Reedy, 1995; Phillips et al., 2001; Yoshimori et al., 2003).
A number of investigators working during the weapons test era reported the
above ground nuclear devices (Drevinsky et al., 1964; Goel et al., 1959; Lal et al., 1960b,
6
Lal et al., 1979). Production of 7Be through nuclear detonations is possible via several
reactions, though the 6Li(d, n)7Be reaction is considered most probable (Drevinsky et al.,
1964). The constituents for this reaction are present only in the fusion charge of a
7
thermonuclear device. Be in precipitation and surface air was found by several
(Arnold and Al-Salih, 1955; Cruikshank et al., 1956; Goel et al., 1959; Lal et al., 1960b;
Rama Thor and Zutshi, 1958). However, measurements made on stratospheric air suggested
7
a possible artificial source. Bleichrodt (1962) reported a fivefold increase in Be
concentrations in the stratosphere over the Netherlands following the start of the 1961
Soviet test series. This increase was seen to be in proportion to the amount of artificial
strontium-89 also present in the stratosphere. A similar observation was again made after
the 1962 Soviet test series (Bleichrodt and Van Abkoude, 1963a). Drevinsky et al. (1964)
attempted to identify bomb-produced 7Be above the natural level in stratospheric air over
the central United States by comparing measured activity concentrations with values
obtained from theoretical calculations of its cosmogenic production. They noted a small
increase above the theoretical range only during the period of the United States nuclear test
the same transport and deposition processes governing the aerosol, making it a useful
atmospheric tracer (Brost et al., 1991; Koch et al., 1996; Koch and Rind, 1998; Rehfeld and
Heimann, 1995). The 7Be-bearing aerosol is thought to be generated through the process of
attachment when 7Be in the form BeO or BeOH adsorbs electrostatically to atmospheric
dust particles (Arnold and Al-Salih, 1955; Lal and Peters, 1967). Transformation of this
aerosol as it traverses the atmosphere can occur through a number of physical, chemical and
meteorological processes (e.g. coagulation of ultra-fine particles, fog and cloud droplet
7
formation, evaporation and condensation, washout, rainout and sedimentation, and
contributions of dust storms and combustion products to the tropospheric aerosol mixture)
which determine the overall activity size distribution of 7Be on the surface air aerosol
population (Winkler et al., 1998). Experimental measurements with cascade impactors (low
flow-rate multistage size fractionating aerosol collection devices) indicate that 7Be-bearing
aerosols in surface air follow a unimodal lognormal size distribution and have an activity
median aerodynamic diameter between about 0.4 and 1.2 µm (Bondietti et al., 1988; El-
Hussein and Ahmed, 1994; Lange, 1994; Papastefanou and Ioannidou, 1995; Papastefanou
by Koch et al. (1996) from a general circulation model. They used the ratio between the
average 7Be content of the troposphere and 7Be depositional fluxes provided by the model
for different latitudinal zones and reported a global average value of 21 days.
Comparatively shorter residence times (approx. 10–15 days) were determined for the
tropics where higher rates of convective circulation and precipitation occur. In the dry
subtropics and polar regions they determined mean tropospheric residence times to be
relatively long (approx. 25–40 days). Mean residence times of 7Be-bearing aerosols in the
troposphere have also been calculated by several other investigators through a variety of
methods and values in the range from around 3 days to greater than 60 days are reported in
the literature (Bleichrodt, 1978; Ďurana et al., 1996; Lal et al., 1960b; Papastefanou, 2006;
Papastefanou and Ionnidou, 1995; Rangarajan and Eapen, 1990; Shapiro and Forbes-Resha,
1976; Rama Thor and Zutshi, 1958; Winkler et al., 1998; Yu and Lee, 2002).
Aerosol residence times in the stratosphere are much longer than for the
troposphere and a residence half-time of the order of 1 year has been reported (Staley,
1982; Thomas et al., 1970). Because this residence time is much longer than the 7Be half-
8
life, equilibrium between the rate of cosmogenic production and radioactive decay of this
stratospheric air indicates an average 7Be concentration in the lower stratosphere in the
range from approximately 150 to 200 mBq m-3 (Dutkiewicz and Husain, 1985; Jordan et al.,
production and loss between the stratosphere and troposphere, there is a fairly high 7Be
concentration gradient between the lower stratosphere and the surface air. Jordan et al.
(2003) reported a mean 7Be concentration in upper tropospheric air of 83 mBq m-3, and
surface air concentrations averaging a few milli-becquerels per cubic metre are widely
different locations worldwide and over different time periods. Table 2.1 summarises a
number of recent and historical studies. Low average concentrations are reported at high
latitude sites, as well as at sites in the Pacific under the intertropical convergence zone.
Hemisphere. Measurements of surface air 7Be concentration have also been made at a large
number of sites in the Americas, as well as at selected sites in the Pacific, Africa and
Antarctica by the Environmental Measurements Laboratory (EML) through its Surface Air
Sampling Program. These data are presently available and show a range in average surface
frequencies below the synoptic variability (Gerasopoulos et al., 2003; Koch and Mann,
1996; Talpos et al., 2005). Seasonal variations in the surface air concentration of this
radionuclide are widely reported in the literature (see, e.g., Al-Azmi et al., 2001; Azahra et
al., 2003; Cruikshank et al., 1956; Feely et al., 1989; Ioannidou et al., 2005; Parker, 1962;
9
Table 2.1. Average surface air concentrations of 7Be at different locations. Data is sorted in order of descending latitude.
7
Location Latitude Be Period Reference
(mBq m-3)
(mBq m-3)
(mBq m-3)
Oahu HI, United States 21°N 3.1 1985 Uematsu et al. (1994)
New Caledonia, South Pacific 22°S 3.1 1985 Uematsu et al. (1994)
Norfolk Island, South Pacific 29°S 2.7 1985 Uematsu et al. (1994)
Hokitika, New Zealand 42°S 3.1 1985–1986 Harvey and Matthews (1989)
Thomas et al., 1970). Feely et al. (1989) found that seasonal variations showed the effects
of at least four factors: (1) stratosphere-to-troposphere exchange (STE); (2) vertical mixing
within the troposphere; (3) air mass transport from middle to high latitudes; and (4) rainfall.
STE is a means for highly concentrated 7Be air from the stratosphere to enter the
troposphere and is generally most intense at middle latitudes during the spring season.
investigators (see, e.g., Appenzeller et al., 1996; Baray et al., 2000; Borman, 1980;
Danielsen, 1968; Danielsen and Mohnen, 1977; Jordan et al., 2003). Vertical mixing of air
within the troposphere can occur through convective circulation. Solar heating of earth’s
surface in the warmer months leads to an increase in temperature of the surface air. Cooler
air sinks and displaces the warm surface air, bringing with it higher concentrations of 7Be
from the upper troposphere. Feely et al. (1989) found the effects of STE and vertical mixing
within the troposphere on seasonal variations of 7Be in surface air to be evident at middle
latitudes, where surface air concentrations of this radionuclide typically show a spring-
summer peak and an autumn-winter trough. Other investigators have also attributed the
observed seasonality at middle latitude sites to a combination of these two factors (Azahra
et al., 2003; Ďurana et al., 1996; Ioannidou et al., 2005). A distinct peak in surface air 7Be
concentrations at Antarctica is reported to occur in the austral summer (Feely et al., 1989;
Lambert et al., 1990). Feely et al. (1989) found that variations in 7Be concentration at the
South Pole paralleled the variations in aerosol concentration with a presumed middle
latitude source. Such air mass transport within the troposphere from middle to high
latitudes is possible through the polar cell of global circulation. Washout by rainfall strips
the surface air. Negative correlations between surface air 7Be concentrations and rainfall
were reported by Feely et al. (1989) for sites where a strong seasonal variation in the
rainfall was observed. Overall, the timing and magnitude of seasonal variations in surface
13
air 7Be concentrations can change with geographical location depending on the contribution
The solar modulation of cosmic-ray fluxes also causes low frequency variations in
the concentration of 7Be in surface air. These variations are noticeable in measurements
made over extended periods and show an anti-correlation with sunspot number (Aldahan et
al., 2001; Cannizzaro et al., 2004; Gerasopoulos et al., 2003; Megumi et al., 2000;
Papastefanou and Ioannidou, 2004). Hötzl et al. (1991) and Megumi et al. (2000) reported
maximum average concentrations of 7Be in surface air to be around 1.6 times higher than
(Germany) and Osaka (Japan), respectively. Koch and Mann (1996) used a Fourier
transform analysis to identify patterns of significant temporal variability in surface air 7Be
concentration measurements of the EML. They found that the amplitude of solar variations
differed between different locations, with no apparent latitude or altitude trends. Also,
highest concentrations of 7Be in surface air at the South Pole occurred along the descending
branch of the sunspot maximum, which they suggested may be the result of low-energy
solar particles being able to penetrate the weaker strength magnetic field above the Poles.
by Zanis et al. (1999) and Gerasopoulos et al. (2001) at a number of alpine stations. They
found episodes of high 7Be concentration to be associated with upper-level ridges and
episodes of low 7Be concentration to be associated with upper-level troughs. Downward air
mass transport from the upper troposphere under anti-cyclonic conditions (upper-level
ridge) and wet scavenging of 7Be-bearing aerosols under the influence of an upper-level
trough were reported by these authors to be the main processes controlling short-term (day-
to-day) variations in surface air 7Be concentrations. Yoshimoro (2005b) suggested that high
weekly 7Be concentrations in the surface air at Tokyo (Japan) may be the result of
downward air mass transport in the troposphere caused by travelling anticyclones formed
between the ridge and trough of the Rossby waves (large-scale meanders of the jet stream).
14
2.9 Deposition
7
Be-bearing aerosols can reach the ground under clear sky conditions through
particle sedimentation (dry deposition), but are removed more efficiently from the
show that around 90 % or more of total 7Be deposition in temperate zones generally takes
place through the wet deposition process (Benitez-Nelson and Buesseler, 1999; Brown et
al., 1989; Fogh et al., 1999; Harvey and Matthews, 1989; Ioannidou and Papastefanou,
2006; McNeary and Baskaran, 2003; Todd et al., 1989; Wallbrink and Murray, 1994). Wet
deposition of 7Be occurs through both below-cloud scavenging (washout) and in-cloud
scavenging (rainout) of its carrier aerosol during a precipitation event. Washout occurs
during the early stages and quickly cleanses the lower troposphere of 7Be-bearing aerosols.
Rainout delivers 7Be from within the cloud layer to Earth’s surface and is active throughout
the duration of a precipitation event. Serial sampling within individual storms shows the
specific activity of 7Be in precipitation to decrease sharply during the initial stages and then
remains fairly constant throughout the mid-to-latter stages, reflecting a change from
washout to rainout as the predominant wet deposition process (Ioannidou and Papastefanou,
Annual deposition of 7Be worldwide ranges from around 400 to 6500 Bq m-2 and
appears to be dependent upon rainfall (Table 2.2). Low annual depositions of this
radionuclide have been reported for sites in the Middle East and Mediterranean regions, as
well as at East Antarctica. The highest annual deposition of 7Be to be reported (6350 Bq
m-2) is for a high rainfall area on the South Island of New Zealand. Young and Silker
(1980) reported an average 7Be flux across the surface of the North Pacific and North
Atlantic oceans of 270 atoms m-2 s-1, which corresponds to an annual deposition of
approximately 1290 Bq m-2. Wallbrink and Murray (1994) are the only investigators to so
far report on 7Be deposition in Australia. They measured an annual deposition of 1030 Bq
15
Table 2.2. Annual 7Be deposition and rainfall at different locations. Data is sorted in order of ascending annual rainfall.
7
Location Latitude Be deposition Rainfall Period Reference
Thessaloniki, Greece 40°N 736 424 1987–1992 Ioannidou and Papastefanou (2006)
Bavaria, Germany 49°N 990 616 1989 Bachhuber and Bunzl (1992)
16
Canberra, Australia 35°S 1030 660 1988–1989 Wallbrink and Murray (1994)
Heidelberg, Germany 49°N 1250 810 1960–1961 Schumann and Stoeppler (1963)
Rijswijk, Netherlands 52°N 1574 881 1961–1961 Bleichrodt and Van Abkoude (1963b)
College Station TX, United States 30°N 2117 980 1990–1990 Baskaran et al. (1993)
Solomons MD, United States 38°N 2080 1112 1986–1987 Dibb (1989)
Fayetteville AR, United States 36°N 867 1156 1980–1984 Lee et al. (1985)
Galveston TX, United States 29°N 2451 1167 1989–1991 Baskaran et al. (1993)
Oak Ridge TN, United States 36°N 2017 1251 1982–1984 Olsen et al. (1985)
17
Stillpond MD, United States 39°N 2167 1260 1995–1996 Kim et al. (2000)
Norfolk VA, United States 36°N 2075 1313 1983–1984 Todd et al. (1989)
Milford Haven, United Kingdom 51°N 1618 1328 1959–1961 Peirson (1963)
New Haven CT, United States 41°N 3780 1390 1977–1978 Turekian et al. (1983)
Hokitika, New Zealand 42°S 6350 2634 1985–1986 Harvey and Matthews (1989)
Table 2.2 (continued).
7
Location Latitude Be deposition Rainfall Period Reference
East Antarctica 70°S 700 n.a. n.a. Nijampurkar and Rao (1993)
North Pacific and Atlantic Oceans 0–60°N 1290 n.a. n.a. Young and Silker (1980)
18
m-2 at Canberra ACT for a corresponding rainfall of 660 mm. Zonal annual average 7Be
deposition has been simulated in a global climate model by Brost et al. (1991). They found
deposition minima to occur in relatively dry regions such as at high latitudes, across the
deserts of northern Africa and the Middle East, and under the subtropical high pressure
systems off the west coasts of the Americas, Africa and Australia. Deposition maxima were
found to occur in regions of relatively high precipitation such as at middle latitudes and
different locations show a high positive correlation with rainfall, and temporal variations in
the depositional flux of this radionuclide generally follow the local rainfall pattern
(Bachhuber and Bunzl, 1992; Baskaran et al., 1993; Benitez-Nelson and Buesseler, 1999;
Caillet et al. 2001; Dueñas et al., 2002; Ioannidou and Papastefanou, 2006; Kim et al.,
2000; Knies et al., 1994; McNeary and Baskaran, 2003; Olsen et al., 1985; Othman et al.,
1998; Turekian et al., 1983). Seasonal changes in the 7Be budget of the troposphere may
also influence the depositional flux of this radionuclide. Dibb (1989) reported the bulk of
7
Be deposition during 1986 and 1987 at Solomons MD (Unites States) to occur during
spring and early summer. This was in spite of near-drought conditions in the spring of
1986. He found the timing of the observed peak in 7Be deposition to be in close agreement
with estimates of the seasonal injection of 7Be rich stratospheric air into the troposphere
due to STE and concluded that the 7Be depositional flux closely reflected the tropospheric
inventory of this radionuclide. Investigators working at other sites across the eastern United
States have also reported springtime maxima in 7Be depositional fluxes (Olsen et al., 1985;
Todd et al., 1989). A pronounced winter peak in the depositional flux of 7Be has been
observed at a number of sites in Japan located along the coast of the Japan Sea (Narazaki et
al., 2003; Yamamoto et al., 2006). Yamamoto et al. (2006) suggested that the flow of cold
air masses containing high 7Be concentration from high latitudes, mixing and generation of
19
convection clouds over the Sea of Japan, and accompanying heavy winter snowfalls were
The deposition velocity of 7Be-bearing aerosols can be calculated from the ratio of
the 7Be depositional flux to its concentration in surface air. Average deposition velocities of
this radionuclide at different locations, including over the Pacific and Atlantic oceans, are
reported to be in the range from 0.004 to 0.074 m s-1 (Crecelius, 1981; Fogh et al., 1999;
Harvey and Matthews, 1989; Papastefanou et al., 1995; Todd et al., 1989; Turekian et al.,
1983; Young and Silker, 1980). Since certain artificial radionuclides (e.g. strontium-90 and
caesium-137) are also found attached predominantly to submicron-sized aerosols and are
present mainly in the stratosphere, the deposition velocity of 7Be may be a useful parameter
(Harvey and Matthews, 1989). This may be especially applicable to Australia and the South
Pacific region, where the distance from major nuclear installations means that any
radioactive pollution is likely to be mixed throughout the troposphere after it descends from
the stratosphere.
They mapped 7Be surface water concentrations and areal activity densities for large areas of
the Pacific and Atlantic oceans and report concentrations in the range from 1 to 12 Bq m-3
and total areal activity densities in the range from 80 to 600 Bq m-2. They found that
concentrations and areal activity densities were higher in areas associated with high rainfall,
and generally increased with latitude. Depth profiles of 7Be were also reported by these
authors and showed that the vertical distribution of this radionuclide in surface ocean
waters generally reflected the temperature profile of the water column. In areas where a
strong thermocline was present within the surface 100 m, they found 7Be concentrations in
the mixed layer to be generally constant and then decrease rapidly below the thermocline.
20
In areas where the thermocline was at a depth of around 100 m or greater, they found 7Be
concentrations to drop to very low values within the mixed layer itself. Concentrations and
depth profiles of 7Be in surface ocean waters were also reported by Silker in a number of
The areal activity density of 7Be in surface soils and grasses is the net result of
deposition, mobilisation, and radioactive decay. Some areal activity densities of this
radionuclide in soils and grasses which have been reported in the literature are summarised
in Table 2.3. Soils with an overlying grass cover seem to maintain a higher 7Be areal
activity density than bare soils, indicating that surface vegetation is an effective trap for
7
Be-bearing aerosols. Bettoli et al. (1995) found more than 50 % of the total 7Be areal
activity density to be present within the grass layer for a number of samples collected at
Bologna (Italy). Wallbrink and Murray (1996) reported local spatial variations in the areal
They attributed this finding to differences in effective fallout and mobilisation of 7Be over
the measurement site prior to its sorption to the soil grain or grass. Local spatial variability
in the areal activity density of other fallout radionuclides (e.g. caesium-137 and
unsupported lead-210) has also been reported for relatively stable sites (Huh and Su, 2004;
Wallbrink et al., 1994; Walling et al., 2003). Temporal variations in 7Be areal activity
densities at undisturbed sites are likely to occur where a seasonal rainfall pattern exists
(Wallbrink and Murray, 1996). The rate of accumulation of this radionuclide is likely to
exceed the rate of loss by decay during months of higher rainfall, while the 7Be half-life
(radioactive decay) will control the areal activity density during months of lower rainfall.
These spatial and temporal variations in areal activity density may affect the use of 7Be as a
tracer in soil movement studies, in particular the selection and sampling of a suitable
reference site.
21
Table 2.3. Total 7Be areal activity densities at undisturbed sites. Data is sorted in order of ascending sampling date.
7
Sampling location Latitude Sample analysed Be areal activity Reference
07/1984 Oak Ridge TN, United States 36°N Grass + soil 673±22 Olsen et al. (1985)
01/1985 Wallops Is. VA, United States 38°N Vegetated marsh soil 673±48 Olsen et al. (1985)
01/1985 Wallops Is. VA, United States 38°N Unvegetated marsh soil 107±19 Olsen et al. (1985)
09/1988 Canberra ACT, Australia 35°S Grass + soil 202±57 Wallbrink and Murray (1996)
09/1988 Canberra ACT, Australia 35°S Bare soil 135±9 Wallbrink and Murray (1996)
22
05/1989 Canberra ACT, Australia 35°S Grass + soil 400±144 Wallbrink and Murray (1996)
05/1989 Canberra ACT, Australia 35°S Bare soil 156±42 Wallbrink and Murray (1996)
08/1989 Canberra ACT, Australia 35°S Grass + soil 205±105 Wallbrink and Murray (1996)
08/1989 Canberra ACT, Australia 35°S Bare soil 95±9 Wallbrink and Murray (1996)
01/1991 Bologna, Italy 44°N Grass + soil 198±9 Bettoli et al. (1995)
01/1991 Bologna, Italy 44°N Bare soil 125±8 Bettoli et al. (1995)
03/1991 Bologna, Italy 44°N Grass + soil 157±8 Bettoli et al. (1995)
Table 2.3 (continued).
7
Sampling location Latitude Sample analysed Be areal activity Reference
03/1991 Bologna, Italy 44°N Bare soil 153±13 Bettoli et al. (1995)
05/1996 West–central Idaho, United States 44°N Grass + soil 139±22 Bonniwell et al. (1999)
01/1998 Crediton, United Kingdom 50°N Bare soil 512±10 Blake et al. (2002)
10/1998 Silverton Mill, United Kingdom 50°N Bare soil 283±26 Blake et al. (2002)
05/1999 Treynor IA, United States 41°N Bare soil 121±21 Wilson et al. (2003)
23
1997–2000 Chintiangang, Taiwan 25°N Grass + soil 3280±1738 Huh and Su (2004)
Because of its short half-life 7Be does not usually penetrate deep into the soil
profile. The activity concentration of this radionuclide in the soil at undisturbed sites
generally shows an exponential decrease with depth (Huh and Su, 2004; Wallbrink and
Murray, 1996, Wilson et al., 2003). Wallbrink and Murray (1996) found 7Be to penetrate no
deeper than 20 mm in soils under various surface cover conditions and reported penetration
half-depths (i.e. the depth at which the activity concentration decreases to half some initial
value) for this radionuclide to be in the range from 0.4 to 3.7 mm. They also found 7Be
concentration to be higher at greater depths in grass covered soils than in bare soils. Olsen
et al. (1985) reported 7Be to a depth of 100 mm in unsaturated marsh soils at Wallops
Island VA (United States). They suggested that particles mobilised by infiltrating rainwater
and transported through small cracks in the soil surface formed during relatively dry
periods might account for this finding. Wallbrink and Murray (1996) concluded that 7Be
cover, soil density, and structure. They also suggested that the incorporation of 7Be into
plant tissue, followed by redistribution along nutrient pathways within the root matrix or
bioturbation by soil fauna could increase the penetration depth of 7Be within the soil
profile.
several reasons: (1) its source is known and global in extent; (2) it has a relatively short
half-life; (3) it attaches rapidly and indiscriminately to available aerosols; (4) it has a steep
concentration gradient between the lower stratosphere and the surface air; (5) it is relatively
simple and inexpensive to measure; and (6) there is a large amount of reliable data available
for hypothesis testing. 7Be measurements have been used by a number of investigators to
test and validate the results of general circulation models of the atmosphere (Brost et al.,
1991; Koch et al., 1996; Rehfeld and Heimann, 1995). The potential for using 7Be to study
24
atmospheric transport processes is particularly great when it is coupled with a nuclide with
a contrasting source function and/or a different half-life. Raisbeck et al. (1981) and Jordan
et al. (2003) demonstrated that the ratio of beryllium-10 (10Be) to 7Be can be used as a
probe of atmospheric transport processes, in particular STE. The source function of 10Be in
the atmosphere is identical to that of 7Be, but its half-life is very much longer (approx.
1.5×106 years). In addition, both radionuclides attach to aerosols and are transported and
deposited in the same way. The production ratio of 10Be/7Be in the atmosphere is reported
by Lal and Peters (1967) to be around 0.5. Levels of 7Be within an irradiated air mass will
reach a relatively steady state within a period of approximately 1 year. However, the
10
Be/7Be ratio will continue to increase over time due to production of 10
Be. Aerosol
residence times in the stratosphere are sufficiently long for this to occur and consequently
10
the ratio of Be/7Be in stratospheric air is higher than in tropospheric air, making the
10
Be/7Be ratio a sensitive indicator of air mass origin and age. The ratio of 10Be/7Be in the
troposphere is reset to its initial production value (i.e. approx. 0.5) following a precipitation
event. Rehfeld and Heimann (1995) and Koch and Rind (1998) simulated 10Be/7Be ratios in
general circulation models to investigate the seasonal and latitudinal changes in STE and air
10
mass transport within the atmosphere. Dibb et al. (1994) measured the Be/7Be ratio in
surface air at Alert NT (Canada) to be nearly constant at 2.2 throughout the year and on the
basis of this finding concluded that the stratosphere was an important source of Be isotopes
source of a scavenged air mass is oceanic versus continental and/or upper versus lower
tropospheric (Baskaran et al., 1993; Benitez-Nelson and Buesseler, 1999; Koch et al.,
210
1996). Pb is a decay product of gaseous radon-222, which emanates primarily from the
surface of continental land masses. Production rates of 7Be in the atmosphere increase with
submicron-sized aerosols and are removed from the atmosphere through similar processes.
25
A relative increase in the 7Be/210Pb ratio can indicate either an upper tropospheric source or
changes in the extent of continental versus oceanic air. At locations where a high
used as two independent atmospheric tracers. Such a correlation has been observed mainly
at continental sites and those close to the continental margin (Baskaran et al., 1993; Hirose
et al., 2004; McNeary and Baskaran, 2003; Todd et al., 1989). Baskaran et al. (1993) found
that 7Be and 210Pb could be used to independently trace air mass origin only at oceanic and
a few coastal sites. Baskaran (1995) reported a seasonal variation in the 7Be/210Pb ratio at
two sites in Texas (United States) during 1990. He concluded that higher values in the
warm summer season were the result of vertical mixing (convective circulation) within the
troposphere, which forces 210Pb enriched (7Be depleted) surface air upward and carries 7Be
surface air show similar seasonal variations as 7Be (Gustafson et al., 1961; Peirson, 1963;
Rangarajan and Gopalakrishnan, 1970; Schumann and Stoeppler, 1963; Thomas et al.,
1970). Artificial radionuclides which are retained in the troposphere following an above
ground nuclear detonation are deposited within a few weeks of their release due to the short
residence time of tropospheric aerosols. Their presence in the troposphere after this time is
due to STE. Alonso Hernandez et al. (2004) used the ratio of 7Be in surface air at
Cienfuegos (Cuba) to 7Be in surface air at Miami FL (United States), as well as caesium-
137 (137Cs) concentrations measured in surface air at Miami, to reconstruct the monthly
137
Cs signal in surface air at Cienfuegos due to global fallout between 1957 and 1994. They
137
found the calculated Cs values for Cienfuegos to be in agreement with measured
concentrations reported for other sites in the Antilles and Central America during the same
epoch. Lee et al. (1985) used the ratio of strontium-90 (90Sr) to 7Be measured in
90
precipitation samples to estimate the amount of excess Sr deposited at Fayetteville AR
(United States) from the 25th Chinese nuclear test explosion. They found that an areal
26
90
activity density of Sr of approximately 13 Bq m-2 was attributable to his event. These
investigators also used polonium-210 (210Po) to 7Be ratios to estimate the amount of excess
210
Po deposited as a result of the May 1980 eruption of Mount St. Helens.
Measurement of 7Be areal activity density and its depth distribution in the soil has
the potential to tell the degree to which the soil surface has been disturbed. Several
investigators have recently used 7Be to document rates of short-term and event-based soil
redistribution (Blake et al., 1999; Blake et al., 2002; Walling et al., 1999; Wilson et al.,
2003). A quantitative estimate of soil erosion is usually made by comparing the areal
activity density within the study area to that measured at a nearby undisturbed and stable
reference point. Wilson et al. (2003) used a 7Be inventory balance to estimate soil erosion
(United States). The inventory balance method accounted for 7Be deposition, losses to
erosion, and changes in areal activity density within the soil profile over the sampling
period. They found that the erosion rate calculated from the 7Be inventory balance
(0.58±0.33 kg m-2) was in agreement with that determined from the sediment flux at the
to relate suspended sediment to its original soil depth (Matisoff et al., 2002; Wallbrink et
al., 1999). 7Be is typically concentrated in the very upper layers, while 137
Cs and
210
unsupported Pb penetrate to deeper layers of the soil profile. Suspended sediment with
relatively high concentrations of all three radionuclides is most likely indicative of a surface
Wallbrink and Murray (1993) used 7Be, 137Cs and unsupported 210Pb to distinguish between
erosion processes during run-off experiments in a field study at Goulburn NSW (Australia).
They found the concentration of all three radionuclides in the suspended sediment to be
initially high, but with the passage of time they observed a decrease in the concentrations of
27
7 210 137
Be and unsupported Pb, while Cs concentration remained constant. They interpreted
this finding as indicating a change from sheet erosion to minor rilling as the dominant
erosion process.
The UNSCEAR reports the annual effective dose due to cosmogenic 7Be to be
0.03 micro-Sieverts (UNSCEAR, 2000). This represents around 0.001 % of the total annual
effective dose received due to all natural radiation sources. Therefore, cosmogenic 7Be does
atmospheric nitrogen and oxygen into lighter fragments. It decays by electron capture to 7Li
spectrometry. 7Be quickly becomes an aerosol associated species and attaches mainly to
particles in the submicron size range. These aerosols have an average residence time in the
this difference in residence time, as well as differences in the rate of production and rate of
loss between the stratosphere and troposphere, there is a fairly high concentration gradient
of 7Be in the atmosphere. Concentrations have been measured at different levels of the
atmosphere and show a decrease of around two orders of magnitude between the lower
stratosphere and the surface air. Surface air concentrations of 7Be are around a few milli-
becquerels per cubic metre on average and exhibit characteristic time variations with
frequencies below the synoptic variability. Seasonal variations in surface air concentrations
28
of a number of atmospheric processes, including stratosphere-to-troposphere exchange,
vertical mixing within the troposphere, air mass transport from middle to high latitudes, and
rainfall. Even lower frequency variations result from the solar modulation of the galactic
cosmic-ray flux to Earth over the 11 year period of the sunspot cycle. Depositional fluxes
of 7Be show a high positive correlation with rainfall, but are also dependent upon the
tropospheric inventory of this radionuclide. Deposition of 7Be occurs mainly through wet
scavenging of its carrier aerosol, which delivers 7Be to ocean and land surfaces. 7Be is
generally present in surface ocean waters, as well as in the upper layers of the soil and
overlying vegetation.
7
Be has its applications in the atmospheric and earth sciences. It is a useful
radionuclide for testing and validating general circulation models of the atmosphere, and
when coupled with a radionuclide of different source function and/or half-life has the
potential to provide valuable information on air mass origin and age. 7Be may also serve as
a useful tool to predict fallout of artificial radionuclides from remote sources due to the
term and event-based soil erosion rates, as well as information on erosion processes, can
also be ascertained from 7Be measurements. Most applications of 7Be require a detailed
understanding of its distribution and behaviour within different environmental systems and
Therefore, further work is required if the full potential of this radionuclide as a tracer of
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different surface cover conditions and its potential for describing soil
Wallbrink, P.J., Murray, A.S., Olley, J.M., 1999. Relating suspended sediment to its
original soil depth using fallout radionuclides. Soil Science Society of America
Walling, D.E., He, Q., Blake, W., 1999. Use of 7Be and 137
Cs measurements to document
Walling, D.E., Collins, A.L., Sichingabula, H.M., 2003. Using unsupported lead-210
Wilson, C.G., Matisoff, G., Whiting, P.J., 2003. Short-term erosion rates from a 7Be
Winkler, R., Dietl, F., Frank, G., Tschiersch, J., 1998. Temporal variation of 7Be and 210Pb
41
Yamamoto, M., Sakaguchi, A., Sasaki, K., Hirose, K., Igarashi, Y., Kim, C.K., 2006.
Seasonal and spatial variation of atmospheric 210Pb and 7Be deposition: features of
the Japan Sea side of Japan. Journal of Environmental Radioactivity 86, 110–131.
Yoshimori, M., 2005a. Production and behaviour of beryllium 7 radionuclide in the upper
Yoshimori, M., 2005b. Beryllium 7 radionucleide as a tracer of vertical air mass transport
Yoshimori, M., Hirayama, H., Mori, S., Sasaki, K., Sakurai, H., 2003. Be-7 nuclei
produced by galactic cosmic rays and solar energetic particles in the Earth’s
Young, J.A., Silker, W.B., 1980. Aerosol deposition velocities on the Pacific and Atlantic
oceans calculated from 7Be measurements. Earth and Planetary Science Letters 50,
92–104.
Yu, K.N., Lee, L.Y.L., 2002. Measurements of atmospheric 7Be properties using high-
Zanis, P., Schuepbach, E., Gäggeler, H.W., Hübener, S., Tobler, L., 1999. Factors
42
CHAPTER THREE
a
International Laboratory for Air Quality and Health, School of Physical and Chemical
Australia
b
Environmental Radiochemistry Group, Australian Nuclear Science and Technology
43
STATEMENT OF JOINT AUTHORSHIP
Title
210
Vertical distributions of Pb excess, 7Be and 137
Cs in selected grass covered soils in
Authors
Conducted field work, prepared samples for analysis, analysed and interpreted data, and
wrote manuscript.
Riaz Akber
Original idea, conducted field work, analysed and interpreted data, and offered advice and
Henk Heijnis
44
Abstract
210
Net accumulated areal activity densities and profiles of Pbex, 7Be and 137
Cs in
the surface 10 cm of the soil are reported for eight sites in Southeast Queensland, Australia.
Areal activity densities of 210Pbex and 7Be varied from 1080 to 4100 Bq m-2 and from 176 to
778 Bq m-2 respectively. A significant (p<0.001) portion of the variance (R2>0.99) in their
vertical distributions was explained by depth in the profile using an exponential function.
210
Around 85 % of accumulated Pbex was present in the surface 10 cm of the soil.
Beryllium-7 was mainly confined to the grass and surface 2 cm of the soil. Average
210
penetration half-depths of 3.6 ± 0.2 cm and 0.3 ± 0.1 cm were determined for Pbex and
7 137
Be, respectively. Areal activity densities of global fallout Cs varied from 10 to 361 Bq
m-2. Its signal was well mixed within the surface 10 cm. Comparison of the measured 137Cs
values to the estimated input value for the region (~490 Bq m-2) and profiling of a 1 m deep
soil core suggests a vertical migration of 137Cs over the past decades.
210
The paleo-radon activity flux determined from the Pbex areal activity density
(5.1 ± 0.9 mBq m-2 s-1) was not statistically different to that measured using activated
charcoal cups (5.5 ± 0.4 mBq m-2 s-1), tending to suggest that Southeast Queensland is
210
Keywords: Pbex; 7Be; 137
Cs; Soil; Areal activity density; Penetration half-depth; Radon
45
3.1 Introduction
development over the past decades, a number of nuclear techniques have been developed
for quantitative assessment of soil erosion and sedimentation rates. Among these, 137Cs has
been extensively used to estimate rates of soil erosion (Ritchie and Ritchie, 2005). This
technique compares the 137Cs areal activity density at an eroded site to a nearby undisturbed
210
site to assess the extent of soil loss. Similar methods based on the measurement of Pb
excess (210Pbex) over 226Ra and 7Be have more recently been established (Zapata, 2003).
210
Caesium-137, Pb and 7Be are all highly particle reactive (see Matisoff et al.
(2002) and references therein). Their deposition to earth labels the land surface with a
unique and identifiable radiological fingerprint. Due to differences in their half-life and
fallout history, these radionuclides are suitable for estimating erosion rates over different
137
timescales. Fissiogenic Cs (half-life, 30.2 years) can provide a retrospective estimate of
land erosion rates over the past 30 to 40 years (Zapata, 2003), i.e. since the cessation of
210
large-scale nuclear weapons tests in the atmosphere, lithogenic Pb (half-life, 22.6 years)
offers a means of estimating erosion rates dating back 100 years (Walling and He, 1999;
Walling et al., 2003), and 7Be (half-life, 53.3 days) can provide an estimate of soil loss
associated with a single erosive event (Blake et al., 1999; Wilson et al., 2003).
(Australian Bureau of Statistics, 2005). Coupled to this growth, urban development has
been identified as a key factor which may accelerate erosion rates in Queensland
populous urban areas, legislative land management practices have been introduced. In the
State’s southeast and along much of the coastal stretch rainwater runoff poses the greatest
threat of erosion, especially during summer when high intensity rainfall usually occurs
(Environmental Protection Agency, 2004). For the purpose of monitoring rates of land
erosion in these areas, quantitative and reproducible methods are required. To highlight the
46
possibility of nuclear methods for future estimates of land erosion rates in Southeast
210
Queensland, in particular the potential usefulness of Pbex and 7Be, this paper examines
210
vertical distributions of Pbex, 7Be and 137
Cs in selected grass covered soils in the region.
210 222
In addition, as the main source of Pbex in surface soils is likely to stem from Rn
222
released to the atmosphere, Rn exhalation rates from the ground have also been
210
measured. Comparison of these exhalation rates with the Pbex areal activity density can
provide additional information about the behaviour and fate of 210Pb in the environment.
Soil samples were collected from eight sites along a linear route intersecting the
to Boonah (Figure 3.1). Sites selected for soil sampling were flat open areas having a
uniform grass cover and set in a semi-natural environment showing no apparent signs of
disturbance. The slope of the terrain at each site was measured at several points. Slopes of
less than 2° were generally recorded, though at Clagiraba (Site 4) the slope of the land was
up to 5° at some points. All sites were outside any land areas used for cattle grazing or
other agricultural activities, i.e. the land had not been tilled. Occasionally the grass at these
sites was clipped using mechanical slashers, but the clippings neither collected nor removed
from the site. Visual inspection of the sites suggested no bioturbation of the soil from ant
3.2.2 Soils
Soil texture varied from loamy sand at Southport (Site 1) to silt loam at
Tabragalba (Site 5). Physicochemical properties of the soils (bulk density, moisture content,
quartz and clay mineral content, organic matter content, particle size distribution, pH and
cation exchange capacity) were determined and are shown in Table 3.1.
47
27° S
Australia
Queensland
Brisbane
0 25 50 km
9
28° S
87 6 5 4 3 21
Pacific
Darling Downs Ocean
Figure 3.1. Location of the sampling sites and map of Australia (inset).
48
Table 3.1. Site location, annual rainfall rate, and physical and chemical properties of the soils (moisture content, composition and particle size
Site Locality Geographical position Rainfall Bulk Moisture Composition Particle size pH CEC
Latitude (S) Longitude (E) Quartz Clay Organic <2 2-75 >75
mineralsb matter μm μm μm
1 Southport 27° 58′ 28″ 153° 25′ 02″ 1454(123) 1490 17 67.2 29.9 2.9 2.9 24.9 72.1 5.8 20.0
2 Ashmore 27° 58′ 56″ 153° 23′ 02″ n.a. 1390 33 69.9 21.1 9.0 5.2 50.3 44.5 5.4 24.1
49
3 Nerang 28° 00′ 00″ 153° 19′ 48″ 1458(117) 1590 27 30.1 61.5 8.4 12.4 55.8 31.7 6.1 29.7
4 Clagiraba 27° 59′ 42″ 153° 14′ 12″ n.a. 1700 24 82.8 12.7 4.5 5.6 44.7 49.7 5.0 16.7
5 Tabragalba 27° 59′ 44″ 153° 02′ 36″ 952(104) 1260 19 40.7 47.9 11.4 16.3 71.1 12.6 6.5 37.9
6 Beaudesert 27° 59′ 37″ 152° 58′ 26″ 912(117) 1450 11 54.8 37.3 7.9 2.3 31.2 65.8 6.2 32.8
7 Coulson 27° 57′ 42″ 152° 44′ 53″ n.a. 1550 10 53.6 39.9 6.5 3.2 33.8 63.0 6.0 26.8
8 Boonah 27° 59′ 37″ 152° 41′ 53″ 861(106) 1290 13 37.7 51.4 10.9 9.1 46.6 44.3 6.3 30.7
a
Numbers in parentheses denote the number of years over which the average rainfall rate has been calculated.
b
Clay minerals present in the soil include albite, microcline, kaolinite, illite and montmorillonite.
3.2.3 Soil sampling method
At each site, twelve soil cores of 5 cm diameter were collected from within a plot
area of between 5 and 6 m2. Nine cores were taken to a depth of 5 cm and sectioned in 1 cm
increments, and three cores taken between 5 and 10 cm depth. Soil from within the same
depth interval was pooled to form a single sample. Grass growing at each site was clipped
to the level of the topsoil and collected as a separate sample. All samples were collected in
the penultimate week of May 2003, roughly corresponding to the end of the wet season in
this subtropical climate. Additional soil samples were collected for analysis of physical and
chemical properties.
The soils were weighed to determine bulk density, dried at 90 °C for 48 h, and
reweighed to determine moisture content. Samples were then crushed using a ring-mill
222
grinder, packed into 65 mm plastic dishes, and sealed to prevent the escape of Rn (the
210
gaseous precursor of Pb). An insufficient sample volume of grass existed to fill the
was added to these samples prior to crushing. Once sealed in their geometry, all samples
222
were left for a period of at least three weeks to allow for Rn to acquire secular
226 222
equilibrium with its parent Ra. Gamma emission following decay of short-lived Rn
214 214 226
progeny radionuclides, Pb and Bi, were then used to calculate the activity of Ra
234 234m 238
present in the sample. Similarly, measured activities of Th and Pa represented U
activity. To accommodate for the detection of 7Be, a number of samples were also counted
Sample analysis was performed at the Australian Nuclear Science and Technology
system. The system comprised an active NaI(Tl) suppression annulus, a NaI(Tl) plug
detector and a reverse electrode germanium detector all housed within an inert lead shield.
50
Detector efficiency was 12 % at 46.5 keV (210Pb), 5.7 % at 477.6 keV (7Be) and 2.5 % at
661.6 keV (137Cs). Sample count times varied between 1 and 4 days. Activities of 238
U
137
series radionuclides and Cs were determined by direct comparison with IAEA standard
using soil and grass matrices spiked with a known amount of certified 7Be standard solution
obtained from Brookhaven National Laboratory (United States). All radionuclide activities
reported herein have been decay corrected to the date of sample collection. Quoted
Jimboomba (Site 9) located approximately 20 km north of the soil sampling route (Figure
3.1). On each occasion, twenty four activated charcoal cups of diameter 7 cm were planted
exhaled from the ground was collected over a 1 week period. The physical characteristics of
this site closely matched with the sites selected for soil sampling. The additional feature of
this site was its accessibility over periods of several days to securely leave measurement
Radon-222 activity was determined through the gamma emissions of its short-
214 214
lived progeny, Pb and Bi, which were measured using common NaI(Tl) gamma
spectroscopy techniques. Each sample was counted for a fixed period of 20 minutes (live-
time). A measure of the background count rate and an efficiency calibration of the system
were performed immediately prior to and succeeding counting of the field samples. The
calibration standard had an identical geometry to the field samples – that is activated
226
charcoal spiked with a known amount of a certified Ra solution obtained from
51
3.3 Results
210
3.3.1 Pbex and 7Be areal activity densities
Areal activity densities of 210Pbex and 7Be in the grass and superficial 10 cm of the
soil ranged from 1080 to 4100 Bq m-2 and from 176 to 778 Bq m-2 respectively (Table 3.2).
On average, only a small fraction of 210Pbex (0.7 ± 0.1 %) was present in the grass. A much
larger portion of 7Be (17.6 ± 2.4 %) was associated with this vegetal layer. Our 210
Pbex
results are comparable to values reported by Pfitzner et al. (2004) for undisturbed soils in
northern Queensland (518 to 3411 Bq m-2). Values listed in Table 3.2 represent around 85
210
% of the accumulated Pbex signature at our measurement sites (see below). No previous
measurements of 7Be in Queensland soils are known to exist, and only a small number of
7
Be soil studies have been conducted in Australia. Beryllium-7 areal activity densities
ranging from 110 to 450 Bq m-2 have been reported for grass covered soils at Black
Mountain, Australian Capital Territory and ranging from 90 to 990 Bq m-2 in clear-felled
and 260 to 620 Bq m-2 in undisturbed eucalypt forest soils are reported at St. Helens,
depth of 10 cm, are shown in Figure 3.2. At all sites the cumulative 210Pbex signal increases
with soil depth, but with a decreasing contribution from the lower layers. This signal
appears to extend beyond 10 cm depth. The depth-rate accumulation of 7Be is much more
rapid than that of 210Pbex. Beryllium-7 remains predominantly in the grass and surface 1 cm
of the soil. Only at Clagiraba (Site 4), Tabragalba (Site 5) and Coulson (Site 7) did we
detect its presence below 2 cm depth. Olsen et al. (1985) measured 7Be to a depth of 10 cm
in unsaturated marsh soils in the eastern United States and suggested that particles
mobilised by infiltrating rainwater may be transported through fissures in the soil surface
formed during relatively dry periods. It has also been suggested that the incorporation of
7
Be into plant tissue, followed by redistribution along nutrient pathways within the root
52
Table 3.2. Accumulated 210Pbex, 7Be and 137Cs areal activity density in the surface 10 cm and portion present in grass.
1 Southport 22/5/2003 2180 ± 240 474 ± 68 217 ± 23 0.3 ± 0.2 15.9 ± 2.3 <0.1
2 Ashmore 22/5/2003 4100 ± 310 778 ± 78 89 ± 19 0.3 ± 0.1 9.3 ± 1.3 1.1 ± 0.6
3 Nerang 20/5/2003 1780 ± 320 383 ± 75 10 ± 2 1.3 ± 0.3 22.6 ± 2.4 10.9 ± 3.8
4 Clagiraba 20/5/2003 1770 ± 210 406 ± 40 361 ± 29 0.8 ± 0.1 22.0 ± 2.3 0.4 ± 0.1
53
5 Tabragalba 20/5/2003 2030 ± 220 322 ± 50 273 ± 25 0.3 ± 0.2 26.3 ± 12.9 0.6 ± 0.2
6 Beaudesert 21/5/2003 1080 ± 160 229 ± 27 19 ± 4 1.0 ± 0.3 21.7 ± 3.1 <0.1
7 Coulson 21/5/2003 1450 ± 210 478 ± 72 61 ± 13 0.8 ± 0.2 6.7 ± 1.4 <0.1
8 Boonah 21/5/2003 2090 ± 260 176 ± 33 272 ± 25 0.5 ± 0.2 16.2 ± 3.7 <0.1
1.2
1.0
210Pb activity density
(relative scale)
0.8
Southport
Ashmore
0.6 Nerang
Clagiraba
ex
0.4 Tabragalba
Beaudesert
Coulson
0.2 Boonah
Eq. (1)
0.0
0 2 4 6 8 10
1.2
1.0
7Be activity density
(relative scale)
0.8
0.6
0.4
0.2
0.0
0 2 4 6 8 10
210
Figure 3.2. Pbex (top) and 7Be (bottom) cumulative areal activity density profiles
normalised to unity at 10 cm depth. The solid line indicates the best fitting exponential
given by Equation 3.1 to the data. Error in individual data points is typically 10 %.
54
matrix or bioturbation by soil fauna could lead to the transportation of 7Be to greater soil
⎡ ⎛ ln 2 ⎞⎤
A = Agrass + Asoil ⎢1 − exp⎜⎜ − x ⋅ ⎟⎟⎥ Equation 3.1
⎣ ⎝ Ph ⎠⎦
where Agrass and Asoil are the contribution from the grass and soil respectively to the
accumulated areal activity density (A), and Ph is the penetration half-depth of the
interval (Figure 3.2). Statistical analysis indicates that a significant (p<0.001) portion of the
when Equation 3.1 is applied to the data. This analysis was performed using the software
package DataFit (Version 8.0) obtained from Oakdale Engineering. Penetration half-depths
210
of 3.6 ± 0.2 cm and 0.3 ± 0.1 cm were determined for Pbex and 7Be, respectively. At the
210
sites selected for this study, roughly 85 % of Pbex activity was concentrated in the upper
210
10 cm of the soil. Further to this, Equation 3.1 also predicts that 95 % of Pbex will be
present in the surface 15 cm and 99 % present in the surface 25 cm of the soil. These results
agree with the findings of Matthews and Potipin (1985), who reported more than 90 % of
210
Pbex in the surface 15 cm and a maximum penetration depth of 25 cm in New Zealand
soils. Our result for 7Be compares favourably with Ph values reported by Wallbrink and
Murray (1996a) for eucalypt forest soils (0.30 to 0.37 cm) at St. Helens, Tasmania, but is
somewhat greater than the Ph reported by the same authors for alluvial bare soils (0.057 to
Southport (Site 1) and Ashmore (Site 2), i.e. nearest the coast. This was in opposition to our
55
expectation that coastal sites would exhibit a lower 210Pbex activity than those further inland
222 222
due to a dilution of Rn from mixing with ocean air. Water bodies emit little Rn
(Wilkening and Clements, 1975) and therefore do not contribute significantly to deposited
210
Pbex radioactivity. Areal activity densities of 7Be were also higher at these sites. Because
of its cosmogenic origin 7Be production rates are independent of geography and its
atmospheric concentration over a small area is expected to be more or less the same.
Therefore factors causing spatial variability in 7Be areal activity density will be 7Be
deposition rate and redistribution of the land surface. Since we have specifically chosen
sites where no apparent perturbations have occurred, variations in the measured 7Be areal
activity density should result from variations in 7Be deposition rate alone. Rainfall is known
(Martin, 2003; Turekian et al., 1983; Wallbrink and Murray, 1994). Our sampling sites are
separated by a series of small mountain ranges. Those sites towards the west of the ranges
(Tabragalba (Site 5), Beaudesert (Site 6), Coulson (Site 7) and Boonah (Site 8)) are located
in a region of traditionally lower rainfall than those nearer the coast (Table 3.1). A
significant (p<0.05) positive correlation (R>0.98) between 7Be areal activity density and
total rainfall in the 12 month period preceding sample collection was observed. But the
correlation between 210Pbex areal activity density and long-term annual average rainfall was
210
poor (R=0.29). To substantiate this apparent lack of relationship between Pbex and
3.3.2 Accumulation of 210Pbex on the land surface and 222Rn activity fluxes
time, an estimate of its accumulation rate (B) on the land surface can be made from its areal
λA
B= Equation 3.2
1 − exp(− λt )
56
In this equation λ is the disintegration constant, A is the areal activity density, and t is the
time over which the activity has accumulated. In the situation where the land surface has
remained undisturbed for a time period much longer than the half-life of the isotope
B = λA Equation 3.3
210
Using Equation 3.3, we have calculated the average accumulation rate of Pbex and 7Be
across our measurement sites as being 73 ± 11 Bq m-2 y-1 and 1.9 ± 0.3 kBq m-2 y-1,
respectively. However, it is well known that the deposition rate of 210Pb and 7Be varies with
rainfall (Fogh et al., 1999; Winkler and Rosner, 2000). In Southeast Queensland the
distribution of the annual rainfall follows a seasonal pattern – around 66 % of the yearly
rainfall occurs between November and April (inclusive) and 34 % falls in the period from
May to October. In the case of 210Pb, the seasonal influence of the rainfall on its deposition
rate is likely to be smoothed over the accumulation period (~100 years). The half-life of
7
Be, on the other hand, is considerably shorter than the temporal variations in the annual
rainfall pattern and as a result its areal activity density is expected to display a seasonal
variation. Hence, 7Be areal activity densities given in Table 3.2 should be viewed as
If on a regional scale an equilibrium exists between 222Rn exhaled from the ground
210
and that deposited back in the form of Pb, and this fallout is the dominant source
222
contributing to its excess, then an estimate of the average Rn activity flux (φ) over the
previous 100 years can be made from the 210Pbex areal activity density (APbex) as
222
where λRn is the Rn disintegration constant. Using Equation 3.4 and correcting the
210
measured Pbex signal to its terminal depth, the paleo-radon activity flux has been
calculated as 5.1 ± 0.9 mBq m-2 s-1. Radon-222 exhalation surveys performed on three
separate occasions yielded activity fluxes of 5.8 ± 0.3, 6.4 ± 0.2 and 2.0 ± 0.2 mBq m-2 s-1,
57
respectively. The first two measurements were made under rainfall free conditions and the
third taken during a period of persistent rainfall. Long-term meteorological records indicate
that in the vicinity of Jimboomba (Site 9) rainfall occurs on approximately 25 % of all days
222
in any given year. From this, a rainfall weighted average Rn activity flux of 5.5 ± 0.4
mBq m-2 s-1 has been determined. This value is not statistically different to the paleo-radon
activity flux determined on the basis of the measured 210Pbex areal activity density and tends
to suggest that Southeast Queensland is neither a net source nor a net sink of 210Pb-bearing
Protection Agency, 2004). Temperatures are warm to mild and the weather is generally
controlled by the passage of non-aggressive high- and low-pressure systems with a hint of
tropical influence resulting in higher rainfall during summer. Near surface air mixing
through eddy currents and the quiescent nature of the weather pattern are most likely
responsible for maintaining a balanced atmospheric 210Pb budget across the region.
While good agreement has been found between our retrospective and direct
measurements, there exist a number of complicating factors which can affect paleo-radon
activity flux calculations using Equation 3.4. Such factors not only include the net influx
210
(or out-flux) of Pb-bearing aerosols to (or from) a region, but also soil properties, e.g.
222
moisture and porosity, which can affect Rn retention in surface soils (Tanner, 1964;
210
Tanner, 1980) and consequently the Pbex areal activity density and profile. It could also
210 226
be argued that an excess of Pb activity over Ra in the soil may arise from a loss of
226 226
Ra. Because of the half-lives involved, it is expected that Ra (half-life, 1600 years)
238
will be in secular equilibrium with its long-lived ancestor U (half-life, 4.5×109 years).
226 210 238
Figure 3.3 shows areal activity densities of Ra and Pb plotted against that of U. In
226 238
general Ra values are less than those of U (i.e. fall below the line of equality)
226 210
suggesting that with time some Ra loss has occurred. The Pb values, however, are in
excess of both 226Ra and 238U, indicating that a loss of 226Ra alone cannot justify the values
of 210Pbex which we have measured in the soil. A weak correlation (R=0.60) between 226Ra
58
1000
Pb activity density (Bq m )
-2
800
600
400
210
226
Ra,
200 Ra
210
226
Pb
1:1
0
0 200 400 600 800 1000
238
U activity density (Bq m -2)
Figure 3.3. 226Ra and 210Pb areal activity density plotted against 238U. The solid indicates the
line of equality. Errors in 226Ra, 210Pb and 238U are typically 5, 10 and 10 %, respectively.
59
210
areal activity density and clay mineral content was observed. However, Pbex areal
In Australia, fallout of radioactive debris from above ground nuclear weapons tests
began in the early 1950’s. Between October 1952 and September 1958 the British
conducted a series of nuclear tests at sites on the Australian continent (Marlinga and Emu
Field, South Australia) and also at nearby Trimouille, Christmas and Malden Islands. The
137
accumulated total Cs input at Brisbane, Queensland (Figure 3.1) between 1954 and the
end of 1978 due to global nuclear testing has been estimated as 488 Bq m-2 (Longmore et
al., 1983). At Swan Creek, located in the Darling Downs area of Southeast Queensland
137
(Figure 3.1), Longmore et al. (1983) report the average Cs areal activity density in
undisturbed soils to be 495 Bq m-2. For the purpose of comparison these values have been
decay corrected to the end of May 2003, corresponding to the soil sampling period of the
present study. As our sampling sites are situated between Brisbane and the Darling Downs,
and the number and yield of atmospheric nuclear tests since 1978 has been relatively low, it
137
does not seem unreasonable to assume the accumulated total Cs input at sites along our
361 Bq m-2 (Table 3.2). These values are at least one order of magnitude less than the
210
corresponding Pbex activity density at each site. Caesium-137 areal activity in grass
surface 10 cm of the soil (Figure 3.4). There was a significant (p<0.001) linear correlation
(R>0.99) between the incremental areal activity density and soil depth. Nerang (Site 3) and
Beaudesert (Site 6) were excluded from this analysis due to an abnormal behaviour. The
137
Cs areal activity density at these sites was lowest among all sites and retained only within
60
1.2
1.0
137Cs activity density
(relative scale)
0.8
0.6
0.4
0.2
0.0
0 2 4 6 8 10
137
Figure 3.4. Cs cumulative areal activity density profiles normalised to unity at 10 cm
depth. The site key is the same as that shown in Figure 3.2. The solid line represents the
best fitting linear function to the data. The dotted lines indicate the 95 % confidence region.
61
210
the surface 2 to 5 cm of the soil. Yet the Pbex signal at these sites exhibited a similar
trend to that observed at other sites (Figure 3.2), suggesting that some surface soil may
137
have been removed from these areas following the cessation of Cs deposition. A Ph for
137
Cs was not determined as the nature of its profile was not exponential, at least within the
surface 10 cm. Analysis of a 1 m deep soil core taken from Jimboomba (Site 9) suggests
137
that the peak in the Cs signature presently resides at a depth of between 10 and 20 cm,
and that at depths greater than 30 cm its activity is below the lower limit of detection.
137
A comparison of our Cs areal activity densities to other values reported in the
137
literature is not offered since we have not quantitatively measured the Cs signal in its
entirety. However, it is apparent from the profile of the deeper soil core and the reduced
areal activity density in the surface 10 cm relative to the estimated input value that a
137 137
vertical migration of Cs has occurred. Such a downward movement of Cs is not
137
uncommon. Schuller et al. (2004) reported the convection velocity of fallout Cs from
global nuclear weapons tests to vary from 0.03 to 0.11 cm y-1 in soils from South Patagonia,
137
Chile. The vertical migration velocity of Chernobyl derived Cs in soils of Western
Macedonia, Greece is reported to be between 0.1 and 0.3 cm y-1 (Arapis and Karandinos,
2004). Caesium-137 sorbs strongly to most soils, particularly to clay minerals. Its
137
downward movement is largely governed by the physical transport of Cs-bearing
particles from the surface to the subsoil layers, though certain physicochemical properties
of individual soils can also affect it mobility (Livens and Loveland, 1988).
3.3.4 Natural radionuclide signatures (210Pbex and 7Be) for use in erosion studies
been dominated by the 137Cs technique. This technique can be used to estimate land erosion
137
rates over the past 30 to 40 years. However, Cs areal activity densities in the Austral
Pacific region have not been replenished since the cessation of above ground nuclear
137
weapon tests. In this region, no significant increase in Cs activity in either surface air
62
(Matthews, 1995) or soil (Schuller et al., 1993) was observed following the Chernobyl
accident. Also, original 137Cs fallouts in the Southern Hemisphere were far less intense than
in the Northern Hemisphere (UNSCEAR, 2000). Forgoing any future weapons test era or
137
serious nuclear accidents, the Cs signal will wane due to both its physical half-life and
dispersion in the soil, thereby restricting its use in future land erosion estimates. If nuclear
methods are to continue to be used as a quantitative means to measure soil erosion, then
Lead-210 and 7Be both have a strong affinity for most soils (Matisoff et al., 2002).
137
But unlike Cs their areal activity densities are continuously replenished through natural
production processes. Applications of these isotopes for studies of land erosion are now
emerging in the literature. For example, Walling and He (1999) and Walling et al. (2003)
used 210Pbex areal activity densities and profiles to estimate rates and patterns of soil erosion
210
on cultivated land. In addition, the results of Walling et al. (2003) demonstrate that Pbex
can be used as an alternative radiotracer to 137Cs for examining erosive soil loss. The work
of Wallbrink and Murray (1996b) indicates that a more sensitive method for investigating
210 137
soil erosion rates is to consider inventory ratios of Pbex to Cs as opposed to either of
these signatures alone. Also, Blake et al. (1999) and Wilson et al. (2003) have shown that
7
Be can be used to quantify rates of water-induced erosion at the event-scale.
The few previous studies of soil erosion and sedimentation rates in Southeast
137
Queensland have focused their attention on the measurement of Cs (Longmore et al.,
1983; Wallbrink, 2004). In this region, no consideration has yet been given to either 210Pbex
or 7Be for quantitative assessment of land erosion rates. The results of the present study
210
demonstrate that Pbex, 7Be and 137
Cs are all present in the surface 10 cm of Southeast
Queensland soil’s and that all three can be simultaneously measured through standard
gamma spectrometric techniques. Given the areal activity profiles which we have measured
and taking into consideration the source of each isotope, i.e. natural and replenished (210Pb
and 7Be) versus anthropogenic and non-replenished (137Cs), it would appear that 210Pbex and
63
7
Be show great promise to be used either individually, together or in conjunction with 137Cs
3.4 Conclusions
Accumulated areal activity densities and profiles of 210Pbex, 7Be and 137Cs in grass
222
covered soils and Rn activity fluxes from the ground have been measured at selected
sites in Southeast Queensland, Australia. The main findings of this study are summarised in
• Areal activity profiles of 210Pbex and 7Be in the surface 10 cm of undisturbed soils
• Average penetration half-depths of 210Pbex and 7Be were determined to be 3.6 ± 0.2
• The vertical distribution and activity of 210Pbex and 7Be indicates that these natural
Acknowledgements
the Australian Institute of Nuclear Science and Engineering in the undertaking of this study
(AINSE grant no. 03/084). We would also like to thank Miss Lindsay Churchley for
carrying out the 222Rn exhalation surveys, Mr. Tony Raftery for the quartz and clay mineral
analysis, Mr. Les Dawes for analysis of additional physical and chemical properties of the
soils, and Mr. Jaya Dharmasiri for preparation of 7Be and 226
Ra calibration standards.
64
Rainfall data used in this study was generously supplied by the Australian Government
Bureau of Meteorology.
References
137
Arapis, G.D., Karandinos, M.G., 2004. Migration of Cs in the soil of sloping semi-
77, 133–142.
Australian Bureau of Statistics, 2005. Regional population growth, Australia and New
Blake, W.H., Walling, D.E., He, Q., 1999. Fallout beryllium-7 as a tracer in soil erosion
Fogh, C.L., Roed, J., Andersson, K.G., 1999. Radionuclide resuspension and mixed
Livens, F.R., Loveland, P.J., 1988. The influence of soil properties on the environmental
Longmore, M.E., O'Leary, B.M., Rose, C.W., Chandica, A.L., 1983. Mapping soil erosion
and accumulation with the fallout isotope caesium-137. Australian Journal of Soil
Martin, P., 2003. Uranium and thorium series radionuclides in rainwater over several
Matisoff, G., Bonniwell, E.C., Whiting, P.J., 2002. Soil erosion and sediment sources in an
Matthews, K.M., 1995. Measurements of residual traces of 137Cs in the atmosphere in New
65
Matthews, K.M., Potipin, K., 1985. Extraction of fallout 210Pb from soils and its distribution
Olsen, C.R., Larsen, I.L., Lowry, P.D., Cutshall, N.H., Todd, J.F., Wong, G.T.F., Casey,
W.H., 1985. Atmospheric fluxes and marsh-soil inventories of 7Be and 210
Pb.
Pfitzner, J., Brunskill, G., Zagorskis, I., 2004. 137Cs and excess 210Pb deposition patterns in
estuarine and marine sediment in the central region of the Great Barrier Reef
102.
Ritchie, J.C., Ritchie, C.A., 2005. Bibliography of publications of 137cesium studies related
http://hydrolab.arsusda.gov/cesium/Cesium137bib2005i.html.
137
Schuller, P., Bunzl, K., Voigt, G., Ellies, A., Castillo, A., 2004. Global fallout Cs
Schuller, P., Løvengreen, C., Handl, J., 1993. 137Cs concentration in soil, prairie plants, and
Tanner, A., 1964. Radon migration in the ground: A review. In: The Natural Radiation
Tanner, A., 1980. Radon migration in the ground: A supplementary review. In: The Natural
Turekian, K.K., Benninger, L.K., Dion, E.P., 1983. 7Be and 210Pb total deposition fluxes at
5411–5415.
UNSCEAR, 2000. Sources and effects of ionising radiation. United Nations Scientific
New York.
66
Wallbrink, P.J., 2004. Quantifying the erosion processes and land-uses which dominate fine
Wallbrink, P.J., Murray, A.S., 1994. Fallout of 7Be in south eastern Australia. Journal of
Wallbrink, P.J., Murray, A.S., 1996a. Distribution of 7Be in soils under different surface
cover conditions and its potential for describing soil redistribution processes.
Wallbrink, P.J., Murray, A.S., 1996b. Determining soil loss using the inventory ratio of
excess lead-210 to cesium-137. Soil Science Society of America Journal 60, 1201–
1208.
Walling, D.E., Collins, A.L., Sichingabula, H.M., 2003. Using unsupported lead-210
Walling, D.E., He, Q., 1999. Using fallout lead-210 measurements to estimate soil erosion
Wilkening, M.H., Clements, W.E., 1975. Radon 222 from the ocean surface. Journal of
Wilson, C.G., Matisoff, G., Whiting, P.J., 2003. Short-term erosion rates from a 7Be
air, atmospheric deposition rate and total deposition velocity in south Germany.
Zapata, F., 2003. The use of environmental radionuclides as tracers in soil erosion and
67
CHAPTER FOUR
AUSTRALIA
68
STATEMENT OF JOINT AUTHORSHIP
Title
Authors
Original idea, collected and prepared samples for analysis, analysed samples, analysed and
Riaz Akber
Assisted with sample collection, assisted with data analysis and interpretation, and offered
69
Abstract
carried out at Brisbane, Australia. Concentrations of 7Be in near-surface air measured over
4 years show seasonal variations with values above the annual mean occurring mainly in
the spring and summer months of each year. These higher concentrations coincide with the
expected influx of stratospheric air to the planetary boundary layer in early spring and
higher rates of convective circulation within the troposphere during summer. 7Be deposition
measurements over 3 years show seasonal variations similar to the seasonal rainfall pattern.
deposition and rainfall amount. This relationship is used to calculate the net cumulative 7Be
70
4.1 Introduction
continuous bombardment of earth’s atmosphere by cosmic radiation (Lal and Peters, 1967).
nucleus of atmospheric nitrogen and oxygen in a process known as spallation. The main
production site of this radionuclide is in the lower stratosphere at a height of around 20 km.
Aircraft and ground based measurements indicate that there is a steep vertical concentration
gradient of 7Be within the atmosphere: concentrations decrease by around two orders of
magnitude between the lower stratosphere and the surface air (Dibb et al., 2003;
and Ioannidou, 1995). Therefore, it is susceptible to the same transport and depositional
processes governing these aerosols, making it a useful atmospheric tracer (Brost et al.,
1991). 7Be labelled aerosols can reach the ground under clear sky conditions through
particle sedimentation (dry deposition), but are removed more efficiently from the
below cloud scavenging (washout) and in cloud scavenging (rainout) of the carrier aerosol.
the Austral Pacific region and also the potential for this radionuclide to quantify rates of
short-term soil erosion. The present study was carried out at Brisbane (Australia) and deals
with the deposition and concentration in near-surface air of cosmogenically produced 7Be.
It examines the temporal variations in each of these quantities and attempts to identify the
processes that cause these variations. Finally, the net cumulative 7Be inventory (areal
activity density) is calculated and compared with values measured in composite grass and
soil samples.
71
4.2 Sampling and analytical techniques
A high volume air sampler (Ecotech, model 2000) and cellulose filter (Whatman,
grade 41) were used to collect aerosol samples from near-surface air. The sampler operated
on a six day cycle (24 hour sampling) and was set up at a height of about 30 m above the
ground level on the roof of the Electrical and Electronic Systems Engineering building at
latitude of 27° 29′ South and a longitude of 153° 2′ East. The air flow rate through the filter
was about 1.17 m3 min-1. The sampler operated from January 2002 until December 2005.
7
Be activity was measured using a well-type high purity germanium detector (Canberra),
which detected the characteristic gamma-ray emission (energy, 477.6 keV) associated with
the transitional electron capture decay of this radionuclide (branching ratio, 0.1044). The
counting efficiency of the detector was determined to be 15.6 % using a certified 7Be
stainless steel funnel that had an effective surface area of approximately 0.57 m2. The
collector was set up directly adjacent to the high volume air sampler. The surface of the
collector was exposed to the atmosphere continuously, thus collecting both wet and dry
directly beneath the collector. At the end of each month, the collector surface and interior
walls of the collection drum were washed with a 1 % nitric acid (HNO3) solution and the
wash added to the sample. The sample was transported to the laboratory in clean
polyethylene buckets and acidified to 1 % HNO3 to prevent any loss of 7Be atoms by
Beaker). The sample was analysed for 7Be activity using a coaxial-type high purity
germanium detector (Ortec). The counting efficiency of the detector was 1.2 % relative to
activity in the sample. Results were decay corrected over the month long sampling period
72
using a half-life of 53.22 days. The uncertainty in monthly measurements was usually less
than 10 %. Measurements were made between January 2004 and December 2006.
The monthly rainfall was obtained from the nearest Bureau of Meteorology
weather station (BOM Station 40913; WMO Station 94576), which was located
Table 4.1. Concentrations which we have measured are similar to those measured
elsewhere at similar latitude (comparative data for a number of sampling sites is available
http://www.eml.st.dhs.gov/databases/sasp).
7
Be concentrations in surface air are sensitive to the phase of the 11-year sunspot
cycle (Koch and Mann, 1996). Therefore, in order to study the behaviour of 7Be in near-
surface air over several years, we have normalised the measured data. Figure 4.1 shows the
percent deviation of monthly average 7Be concentrations away from the annual mean. The
normalised data shows seasonal variations with concentrations above the annual mean
occurring mainly in the spring and summer months (September–February) of each year.
Such variations are a widely recognised phenomenon and are said to be the manifestation of
transport within the troposphere and rainfall (Feely et al., 1989). The increase in 7Be
concentration during the early spring at our sampling site coincides with the circulation of
stratospheric air into the planetary boundary layer based on observations of strontium-90
(90Sr) in surface air at southern latitudes (Rehfeld and Heimann, 1995). 90Sr is an artificial
radionuclide present mainly in the stratosphere except immediately after an above ground
nuclear detonation. The higher concentrations of 7Be in near-surface air throughout the late
73
Table 4.1. Summary of near-surface air 7Be concentration measurements at Brisbane during
50%
2002 2003 2004 2005
25%
Deviation from annual mean
0%
J F MA M J J A S O N D J F M A M J J A S O N D J F M A M J J A S O N D J F M A M J J A S O N D
-25%
-50%
Figure 4.1. Percent deviation of monthly average 7Be concentrations from the annual mean
at Brisbane during the years 2002–2005. Uncertainty in 7Be concentrations is generally less
than 10 %.
74
spring and summer are most likely sustained by higher rates of convective circulation,
bringing 7Be rich air from the upper to the lower troposphere and into the surface air.
Rainfall does not seem to have a controlling influence over the seasonal behaviour of 7Be in
7
4.3.2 Be deposition
Table 4.2 summarises the results of the 7Be deposition measurements. Monthly
values of 7Be deposition and rainfall are shown in Figure 4.2. The temporal pattern in 7Be
Figure 4.3 shows 7Be deposition plotted against rainfall for each month of the
study with the linear least squares regression line representing the empirical relationship
where Y and X represent the monthly 7Be deposition (Bq m-2) and rainfall (mm),
respectively. The coefficient of determination (R2) for this relationship indicated that 72 %
of the variance in 7Be deposition was explained by the variance in rainfall, which was
variance in 7Be deposition was accounted for by the variance in 7Be concentration in near-
surface air. This finding suggests that the deposition of 7Be is not constrained by its
The y-axis intercept of the linear fit shown in Figure 4.3 suggests a monthly dry
deposition component of 35 ± 9 Bq m-2. However, this is around four times higher than the
measured deposition of 9 ± 3 Bq m-2 in July 2004 when only 0.6 mm of rainfall was
recorded. The latter (measured) value suggests that dry deposition of 7Be at our sampling
site constitutes around 10 % of the total deposition of this radionuclide on an annual basis.
The total deposition velocity of 7Be labelled aerosols was calculated as the ratio of
the monthly deposition to the monthly average concentration in near-surface air and ranged
from 0.75 to 25 mm s-1 with a mean of 6.8 mm s-1. By comparison, Young and Silker
75
Table 4.2. Summary of 7Be deposition measurements at Brisbane during the years 2004–
2006.
300
Be deposition (Bq m -2)
200
Rainfall (mm)
100
7
0
J F MA M J J A S O N D J F MA M J J A S O N D J F MA M J J A S O N D
Figure 4.2. Monthly 7Be deposition (columns) and rainfall (solid circles) at Brisbane during
76
300
200
Be deposition (Bq m -2)
7
100
0
0 100 200 300
Rainfall (mm)
Figure 4.3. Monthly 7Be deposition (Y) plotted against monthly rainfall (X). The solid line
77
(1980) determined the average deposition velocity for the standing crop of 7Be over the
South Pacific Ocean to be 9.0 mm s-1 at latitudes between 20°S and 30° S. Changes in the
deposition velocity at our sampling site were most closely linked to changes in the monthly
The net cumulative 7Be areal activity density was calculated from available
monthly rainfall data using the relationship shown in Figure 4.3 by allowing the predicted
areal concentration to decay exponentially and then summing with the concentration from
the next month, and so on (Wallbrink and Murray, 1994). Figure 4.4 shows the calculated
net cumulative 7Be areal activity density and corresponding monthly rainfall at our
sampling site during the years 2000–2006. The 7Be decay curve shows that the areal
activity density will be representative after about 12 months, i.e. when 7Be activity
deposited prior to January 2000 has decayed to less than 1 % of its original value. After 12
months the areal activity density shows distinct seasonal variations that are related to the
seasonal pattern in rainfall. The areal activity density increases sharply during the
maximum rainfall periods which typically occur in the austral summer at our sampling site.
The values are then controlled by the 7Be half-life and subsequent lower intensity rainfall.
The calculated average areal activity density for a period of 6 years (2001–2006) was 310
Bq m-2. The maximum and minimum values during this period were 180 and 540 Bq m-2,
respectively. These variations suggest that the net cumulative 7Be areal activity density at a
measurement site can vary substantially depending upon the time at which samples are
The calculated net cumulative areal activity density was checked on one occasion
(April 2005) against that measured in composite grass and soil samples taken to a depth of
20 mm from an adjacent site. The average 7Be areal activity density of 356 ± 38 Bq m-2
from these samples was around 30 % higher than the calculated areal activity density of 270
78
Table 4.3. Comparison of measured and calculated net cumulative 7Be areal activity
Measured Calculated
600
500
Be decay curve (relative scale)
Areal activity density (Bq m -2)
400
Rainfall (mm)
300
200
7
100
0
J A J O J A J O J A J O J A J O J A J O J A J O J A J O
2000 2001 2002 2003 2004 2005 2006
Figure 4.4. Calculated net cumulative 7Be areal activity density (columns) and measured
rainfall (solid circles) at Brisbane during the years 2000–2006. The solid line is the decay
curve for 7Be activity deposited before January 2000. The dashed line shows the trend in
rainfall.
79
± 46 Bq m-2. It is interesting to note that the site from which the samples were taken used
an automated sprinkler system to water the grounds during dry spells. The system
effectively simulated rainfall in the surface 5–10 m of the air and has probably added to the
total 7Be deposition locally through the washout process, though the actual contribution is
not known. Net cumulative areal activity densities were also calculated for several more
sites in the region where we have previously measured 7Be in composite grass and soil
samples (Doering et al., 2006). Spray irrigation did not occur at these sites. Soil sampling
was performed during May 2003. Rainfall data for each site was obtained from the nearest
Bureau of Meteorology weather station. The results are summarised in Table 4.3 and
indicate that the measured and calculated areal activity densities generally agree within
statistical uncertainties. However, in each case the calculated value is somewhat higher,
suggesting the possibility of overestimation and/or some loss of 7Be from the soil sampling
site.
4.4 Conclusion
7
Be in near surface air was measured over a 4 year period and 7Be deposition
measured over a 3 year period at Brisbane, Australia (lat. 27° 29′ S, long. 153° 2′ E).
Concentrations of 7Be in near-surface air showed seasonal variations with values above the
annual mean occurring mainly in the spring and summer months of each year. These
variations were attributed to the injection of stratospheric air into the surface air in early
spring and increased convective circulation within the troposphere during summer. Levels
of 7Be in near-surface air did not appear to control the amount of deposition of this
radionuclide. Rather, rainfall was found to be an excellent predictor of 7Be deposition with
scavenging was the dominant removal mechanism of 7Be from the troposphere with dry
deposition estimated to comprise around 10 % of the total deposition during any single
year.
80
The net cumulative 7Be areal activity density was calculated from the deposition
and showed seasonal variations that were influenced by the seasonal rainfall pattern. The
average areal activity density measured in composite grass and soil samples taken from a
nearby site was found to be higher than the calculated value. It was suggested that washout
of 7Be at this site may have been increased by the use of an automated sprinkler system. At
other sites in the region where 7Be in grass and soil has previously been measured, the
calculated and measured areal activity densities agreed within statistical uncertainty in most
cases.
References
Brost, R.A., Feichter, J., Heimann, M., 1991. Three-dimensional simulation of 7Be in a
Dibb, J.E., Talbot, R.W., Scheuer, E., Seid, G., DeBell, L., Lefer, B., Ridley, B., 2003.
1–8.
210
Doering, C., Akber, R., Heijnis, H., 2006. Vertical distributions of Pb excess, 7Be and
137
Cs in selected grass covered soils in Southeast Queensland, Australia. Journal of
Dutkiewicz, V.A., Husain, L., 1985. Stratospheric and tropospheric components of 7Be in
Feely, H.W., Larsen, R.J., Sanderson, C.G., 1989. Factors that cause seasonal variations in
9, 223-249.
7
Koch, D.M., Mann, M.E., 1996. Spatial and temporal variability of Be surface
81
Lal, D., Peters, B., 1967. Cosmic ray produced radioactivity on the Earth, in: Sitte, K. (Ed.),
Papastefanou, C., Ioannidou, A., 1995. Aerodynamic size association of 7Be in ambient
Rehfeld, S., Heimann, M., 1995. Three dimensional atmospheric transport simulation of the
210
radioactive tracers Pb, 7Be, 10
Be, and 90
Sr. Journal of Geophysical Research
100, 26141-26161.
Wallbrink, P.J., Murray, A.S., 1994. Fallout of 7Be in South Eastern Australia. Journal of
Young, J.A., Silker, W.B., 1980. Aerosol deposition velocities on the Pacific and Atlantic
Oceans calculated from 7Be measurements. Earth and Planetary Science Letters
50, 92–104.
82
CHAPTER FIVE
83
STATEMENT OF JOINT AUTHORSHIP
Title
Describing the annual cyclic behaviour of 7Be concentrations in surface air in Oceania
Authors
Original idea, collected samples and supplementary data, analysed samples, analysed and
Riaz Akber
Assisted with sample collection, assisted with data analysis and interpretation, and offered
84
Abstract
distinct annual cycle. We apply a sinusoidal model to describe this cycle. The results of
model fitting show that peak 7Be concentrations in surface air occur during early spring at
tropical latitudes and during mid-to-late summer at middle latitudes. Comparison with
90
available Sr surface air data for the southern hemisphere indicates that stratosphere-to-
troposphere exchange is an active atmospheric process controlling the 7Be annual cycle
throughout the Oceania region. Vertical transport of air within the troposphere also seems
to influence the observed annual cycle. Seasonality in rainfall is not thought to control the
85
5.1 Introduction
nucleus of atmospheric nitrogen and oxygen into lighter fragments (Lal and Peters, 1967).
It decays by electron capture to lithium-7 and has a half-life of approximately 53 days. 7Be
useful radionuclide for studying atmospheric transport processes (Brost et al., 1991; Jordan
et al., 2003). Concentrations of 7Be in surface air show characteristic time variations with
frequencies below the synoptic variability (Koch and Mann, 1996). The well reported
annual cycle is said to be the manifestation of several meteorological factors (Feely et al.,
1989). There have been few studies of 7Be in surface air reported for sites in Oceania
(Garimella et al., 2003; Hicks and Goodman, 1977; Uematsu et al., 1994). Most
measurements carried out in the region are of a monitoring nature only, and little
interpretation of the data has been performed. To better understand the annual cycle of 7Be
in surface air and to identify factors that may be controlling this behaviour, we present an
analysis of 7Be surface air concentrations for several stations in the Oceania region.
Laboratory of New Zealand (Matthews, 1996), the University of the South Pacific
station is shown in Figure 5.1 and the time periods over which the measurements were
86
Equator 1
3
4
5
Tropic of Capricorn
6
30° S 7
9 11 10
12
13
150° E 180° E, W 150° W
87
Table 5.1. Location of sampling stations, measurement periods, mean 7Be concentration in surface air, and long-term annual average rainfall.
Latitude Longitude
10 Lower Hutt (New Zealand) 41.2°S 174.9°E 1987–1999 2.9 ± 0.8 1249
Latitude Longitude
The sampling and analytical techniques for most stations have been previously
reported in the literature (see, e.g., Feely et al., 1989; Garimella et al., 2003; Matthews,
1996; Uematsu et al., 1994). We only provide a description of our own methods.
A high volume air sampler (Ecotech, model 2000) and cellulose filter (Whatman,
grade 41) were used for aerosol collection. Air was drawn through the filter at a rate of
approximately 1.17 m3 min-1 over a 24 hour period. Samples were collected at 6 day
intervals. 7Be activity collected on the filter was measured through the characteristic
gamma-ray emission associated with the transitional electron capture decay of this
radionuclide (branching ratio, approx. 10 %). A quarter section of the filter was pressed into
a small pellet and counted on a Canberra well-type high purity germanium detector. The
7
Be counting efficiency of the detector was determined using a certified 7Be standard
purchased from Brookhaven National Laboratory (United States). The concentration of 7Be
in surface air was calculated using the half-life, branching ratio, counting efficiency,
sampled air volume, and time delay in sampling and measurement. Monthly average
concentrations were calculated using the arithmetic mean. The overall uncertainty in
Measurements at different stations were made over different time periods (Table
5.1). Koch and Mann (1996) showed that concentrations of 7Be in surface air are sensitive
to the phase of the sunspot cycle. Lower concentrations typically occur at sunspot
maximum due to a decrease in the galactic cosmic-ray flux to Earth and vice-versa. This is
a global phenomenon. In addition, Koch and Mann (1996) identified a cyclic pattern having
a periodicity of around 2 to 3 years. They suggested that these variations were caused by
low frequency solar and ENSO variations we have normalised the concentration data.
90
Normalised data
Annual cycle
Spectral density (relative scale)
Un-normalised data
Annual cycle
Solar cycle
ENSO cycle
0 1 2 3 4
-1
Frequency (years )
Figure 5.2. Frequency representation of normalised (top panel) and un-normalised (bottom
panel) 7Be concentration data for the monitoring station at American Samoa.
91
Also, as not all detector systems were inter-calibrated, normalising the data may help to
reduce any inconsistencies between the measurement laboratories. The annual mean
concentration was subtracted from the monthly mean concentration of the corresponding
year and then divided by the annual mean to produce a set of monthly deviations from the
annual mean concentration for each year. Figure 5.2 shows the frequency representation of
the normalised and un-normalised concentration data for the monitoring station at
American Samoa, where measurements were made over a period of 24 years. It can be seen
that normalising the concentration data effectively removes the low frequency solar and
ENSO variations.
We wish to describe the annual cycle in surface air 7Be concentrations at each
station using a sinusoidal model similar to that developed by Junge (1963) for describing
synthesized an average year by calculating the mean of monthly deviations for each station.
The model used to describe these deviations is given by Equation 5.1. In this equation, y is
the percent deviation of 7Be concentration away from the annual mean at time t. The
amplitude of the oscillation is given by y0. The phase, φ, indicates the time in months
relative to the start of the calendar year at which peak 7Be concentrations in surface air are
The results of Equation 5.1 applied to the mean of monthly deviations at each
station are presented in Table 5.2 in order of ascending latitude. For each station the
correctness of Equation 5.1 to describe the behaviour of 7Be in surface air, we consider the
92
Table 5.2. Summary of results of sinusoidal model fitting.
93
coefficient of determination and the power of the fit. The coefficient of determination (R2)
is the ratio of the variation explained by the model to the total variation. It is a measure of
the certainty in making predictions from a particular model. The power (P) is the
probability that the model correctly describes the relationship of the variables and is
affected by the level of significance at which the model is tested. Values of R2 and P for
each station are given in Table 5.2. In general, the model shows good statistical rigor. The
amount of variation explained by the model is in the range 59–97 % and the probability that
the model correctly describes the relationship of the variables is in the range 82–99 %. It
therefore seems that factors controlling the annual cycle of 7Be in surface air produce a
The phase of the annual cycle predicted by Equation 5.1 varies between the
stations (Table 5.2). Between tropical latitudes and middle latitudes there appears to be a
delay of up to 5 months in the occurrence of peak 7Be concentrations in surface air. Peak
concentrations occur in early spring at tropical latitudes, during early summer at subtropical
latitudes, and during mid-to-late summer at middle latitudes. Hicks and Goodman (1977)
reported the annual peak in surface air 7Be concentrations to propagate poleward at a rate of
approximately 1000 km month-1 at stations setup along the 150th meridian east between 9°S
and 43°S. Our own analysis suggests that over the whole of the Oceania region such a shift
mainly occurs between 20°S and 35°S. This finding may be explained by a poleward
However, there may also be a difference in the relative importance and timing of the
atmospheric processes controlling the annual cycle between the different stations.
Koch et al. (1996) reported the mean residence time of 7Be-bearing aerosols in the
troposphere to be around 3 weeks. Aerosol residence times in the stratosphere are much
longer than for the troposphere and a residence half-time of the order of 1 year has been
94
reported (Thomas et al., 1970). Because the stratospheric residence time is much longer
than the 7Be half-life, equilibrium between the rate of cosmogenic production and
radioactive decay of this radionuclide is assumed to exist within the stratosphere. Jordan et
al. (2003) reported the average concentration of 7Be in the lower stratosphere to be around
185 mBq m-3. Owing to differences in residence time, as well as rate of production and rate
of loss between the stratosphere and troposphere, there is a fairly high 7Be concentration
gradient between the lower stratosphere and the surface air. Average concentrations of 7Be
in surface air are typically a few milli-becquerels per cubic metre (see, e.g., Brost et al.,
1991). Elevated levels of 7Be in surface air have been used in the past to indicate an upper
atmospheric source (Husain et al., 1977; Viezee and Singh, 1980). However, concentrations
of 7Be in surface air can vary in response to a number of atmospheric processes. Feely et al.
(1989) reported that the annual cyclic behaviour of 7Be in surface air showed the effects of
STE is a means for concentrated 7Be air from the stratosphere to enter the
weapon tests can be used to indicate the presence of stratospheric air in the troposphere (Lal
and Suess, 1968). We can attempt to gauge the effect of STE on the 7Be annual cycle by
comparing the 7Be results with surface air measurements of artificial radionuclides reported
in the literature. Figure 5.3 shows a latitude-time isopleth diagram of the zonal averaged
ratio of the mean of monthly strontium-90 (90Sr) concentrations in surface air for the period
1964–1968 reported by Rehfeld and Heimann (1995). A similar spatiotemporal trend to that
figure. 90Sr concentrations in the southern tropics show a peak in the early spring season.
There is a progressive shift in phase of this peak towards the summer months at latitudes
greater than about 20°S. Peak concentrations of 90Sr in surface air at southern mid-latitudes
can be seen to occur in the mid-to-late summer season. It therefore seems that STE is an
95
This figure is not available online.
Please consult the hardcopy thesis
available from the QUT Library
Figure 5.3. Latitude-time isopleth diagram of the zonal averaged ratio of the mean of
monthly 90Sr concentrations in surface air. From Rehfeld and Heimann (1995).
96
active atmospheric process controlling the 7Be annual cycle at stations in the Oceania
region. As an example of the similar behaviour of both 7Be and 90Sr in surface air, Figure
5.4 shows a plot of mean of monthly 7Be deviations for a number of the measurement
stations and mean of monthly 90Sr deviations at the equivalent latitude. The peak to trough
subsidence of stratospheric air. 7Be on the other hand is produced in both the stratosphere
Vertical transport of air between the upper and lower troposphere can occur
through convective circulation. Solar heating of Earth’s surface in the warmer months leads
to an increase in temperature of the surface air. Cooler air from above sinks and displaces
the warm surface air, bringing with it high concentrations of 7Be from the upper
troposphere. 7Be concentrations in the upper troposphere are the result of in-situ production
as well as STE. Maximum STE in the southern hemisphere is reported to occur in mid-
winter (Appenzeller et al., 1996). Stratospheric air that enters the troposphere must
therefore remain suspended in the upper troposphere for some time before descending to
the surface air. At stations located in the tropics, vertical mixing within the troposphere is
probably quite rapid due to the perpetually warm surface air temperatures above the West
Pacific Warm Pool. However, stations located at more temperate latitudes experience more
distinct warm and cool seasons. Our results show that peak concentrations of 7Be in surface
air at middle latitude stations in Oceania occur in the summer season when surface air
temperatures are also high (Table 5.2). This peak in 7Be coincides with the peak in 90
Sr
concentrations in surface air at these latitudes. It therefore seems that, in addition to STE,
vertical transport within the troposphere is an active atmospheric process which influences
Washout by rainfall removes 7Be-bearing aerosols from the lower troposphere and
decreases the concentration of this radionuclide in surface air. In Oceania, low mean 7Be
concentrations generally occur at stations were the annual rainfall is high (Table 5.1). Most
97
75%
American Samoa (14.3°S)
50%
25%
0%
-25%
-50%
-75%
jan feb mar apr may jun jul aug sep oct nov dec
75%
Brisbane (27.5°S)
50%
25%
0%
-25%
-50%
-75%
jan feb mar apr may jun jul aug sep oct nov dec
75%
Cape Grim (40.7°S)
50%
25%
0%
-25%
-50%
-75%
jan feb mar apr may jun jul aug sep oct nov dec
Figure 5.4. Mean of monthly 7Be deviations (filled circles) at American Samoa (top panel),
90
Brisbane (middle panel) and Cape Grim (bottom panel), and mean of monthly Sr
98
Table 5.3. Values of linear correlation coefficient (R) and Spearman correlation coefficient
(ρ) between mean of monthly 7Be deviations and long-term mean of monthly rainfall.
99
stations experience a seasonal rainfall pattern. Feely et al. (1989) suggested that the rainfall
affecting an air mass prior to its arrival at a sampling site may be better represented by the
long-term mean of monthly rainfall for the site rather than the actual amount of rain falling
in any particular month. This is because an approaching air mass has a good likelihood of
passing through bands of rain producing clouds whether or not such bands happen to
produce rainfall at the sampling site itself. We have calculated the linear correlation
coefficient (R) and Spearman correlation coefficient (ρ) between mean of monthly 7Be and
long-term mean of monthly rainfall at each station. Values of R and ρ are given in Table
between the variables and does not assume the association to be linear. The calculated value
of ρ is significant (p<0.05) for a number of the stations. This finding suggests that the
seasonal pattern in rainfall may also be influencing the 7Be annual cycle. However, the
seasonal pattern in rainfall is perhaps more coincidental with the timing of other processes
(e.g. STE and vertical transport within the troposphere) rather than causal. Stations at
Lower Hutt and Hokitika are located within close proximity but experience different annual
rainfall patterns. Lower Hutt shows a distinct seasonal rainfall pattern, whereas rainfall at
Hokitika is distributed fairly evenly throughout the year. Nevertheless, both stations show a
distinct and in phase 7Be annual cycle. Also, the correlation between mean of monthly 7Be
and mean of monthly rainfall at Invercargill is poor, but a distinct cyclic behaviour of 7Be
5.4 Conclusions
air at a number of stations in the Oceania region. The observed annual cycle of 7Be was
well approximated by a sinusoidal model at most stations. The results of model fitting
100
vertical transport of air from the upper to the lower troposphere were active atmospheric
processes controlling the 7Be annual cycle. A significant (p<0.05) negative correlation
between mean of monthly 7Be and long-term mean of monthly rainfall was found to exist at
with the timing of other atmospheric processes rather than a mechanistic cause of the
Acknowledgements
Tokyo (Japan) and Professor Sitaram Garimella of the University of the South Pacific (Fiji)
References
Appenzeller, C., Holton, J.R., Rosenlof, K.H., 1996. Seasonal variation of mass transport
Brost, R.A., Feichter, J., Heimann, M., 1991. Three-dimensional simulation of 7Be in a
http://www.eml.st.dhs.gov/databases/sasp.
Feely, H.W., Larsen, R.J., Sanderson, C.G., 1989. Factors that cause seasonal variations in
9, 223–249.
Garimella, S., Koshy, K., Singh, S., 2003. Concentration of 7Be in surface air at Suva, Fiji.
Hicks, B.B., Goodman, H.S., 1977. Seasonal and latitudinal variations of atmospheric
radioactivity along Australia’s east coast (150°E longitude). Tellus 29, 182–188.
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Husain, L., Coffey, P.E., Meyers, R.E., Cederwall, R.T., 1977. Ozone transport from
1–3-14.
Junge, C.E., 1963. Studies of global exchange processes in the atmosphere by natural and
Koch, D.M., Jacob, D.J., Graustein, W.C., 1996. Vertical transport of tropospheric aerosols
Lal, D., Peters, B., 1967. Cosmic ray produced radioactivity on the Earth, in: Sitte, K. (Ed.),
Lal, D., Suess, H.E., 1968. The radioactivity of the atmosphere and hydrosphere. Annual
and Rarotonga, in: Akber, R.A., Martin, P. (Eds.), SPERA96: Radioactivity in the
Rehfeld, S., Heimann, M., 1995. Three dimensional atmospheric transport simulation of the
210
radioactive tracers Pb, 7Be, 10
Be, and 90
Sr. Journal of Geophysical Research
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Thomas, C.W., Young, J.A., Wogman, N.A., Perkins, R.W., 1970. The measurement and
pp. 158–172.
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Uematsu, M., Duce, R.A., Prospero, J.M., 1994. Atmosphere beryllium-7 concentrations
Viezee, W., Singh, H.B., 1980. The distribution of beryllium-7 in the troposphere:
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CHAPTER SIX
CONCLUDING REMARKS
The research presented in this thesis advances our knowledge of the distribution
and behaviour of 7Be in the natural environment, particularly within the Southeast
Queensland region of Australia. It has investigated the vertical distribution of 7Be in grass
covered soils and identified factors controlling the areal activity density of this
radionuclide. It has also investigated the atmospheric cycle of 7Be in the troposphere
Areal activity density profiles of 7Be in grass covered soils were obtained for a
number of sites in Southeast Queensland. 7Be was found mainly in grass and the surface 1
cm of the soil. Grass was found to be a good sink for 7Be-bearing aerosols, with around 18
% of the total areal activity density of this radionuclide being present in this vegetal layer
on average. The average penetration half-depth of 7Be in the soil was determined to be 0.3
± 0.1 cm. The measured vertical distribution of 7Be within the soil suggested that this
radionuclide may be suitable for studying erosion and redistribution of surface soils in the
Southeast Queensland region. A high positive correlation existed between 7Be areal activity
density and rainfall amount during the 12 month period preceding sample collection. This
finding suggested that 7Be areal activity densities were subject to temporal variations
Brisbane. The observed temporal pattern in 7Be deposition was seasonal and closely
matched the temporal pattern in rainfall. A high positive correlation between monthly 7Be
deposition and monthly rainfall existed and suggested that wet scavenging was the
dominant removal mechanism of 7Be-bearing aerosols from the lower troposphere. Dry
104
deposition of 7Be-bearing aerosols was estimated to constitute around 10 % of total annual
deposition of this radionuclide on average. There was a poor correlation between monthly
7
Be deposition and mean monthly 7Be concentration in surface air. This finding suggested
that the deposition of 7Be was not constrained by its availability in surface air on a monthly
timescale.
A historical record of 7Be areal activity density extending over several years was
generated from results of the deposition measurements. This record showed that 7Be areal
activity densities at Brisbane varied seasonally and followed the local rainfall pattern. The
areal activity density was found to rise sharply during months of high intensity rainfall and
then decrease at a slower rate in subsequent months governed mainly by the 7Be half-life
and lower intensity rainfall. The results suggested that 7Be areal activity density could
potentially vary by up to a factor of 3 depending on the time when samples were collected
and local rainfall conditions. Comparison of calculated and measured 7Be areal activity
Southeast Queensland.
with 7Be data for a number of additional sites in the Oceania region was performed. The
annual cycle of 7Be in surface air at each site was described using a sinusoidal model. The
proportion of the variance explained by the model was in the range 59–97 % and the
probability that the model correctly described the relationship of the variables was in the
range 82–99 %. The results showed that there was a delay of up to 5 months in the
occurrence of peak 7Be concentrations in surface air between tropical and middle latitudes.
Comparison of the 7Be results with available 90Sr surface air observations for the Southern
annual cyclic behaviour of 7Be in surface air at sites in the Oceania region. Vertical
105
transport of air from the upper to lower troposphere was also identified as influencing the
This thesis has presented measurements and analysis of the distribution and
behaviour of 7Be in a number of natural systems. It adds to the current 7Be knowledge base
and provides a foundation for further study. The next step in research is to use this
problems. One area in particular is the use of 7Be areal activity densities to investigate
erosion and redistribution of surface soils in the Southeast Queensland region. Soil erosion
accelerated rate due to high rates population growth and urban development. Land
management strategies for controlling this loss will require quantitative methods of
assessing erosion rates and processes. Nuclear techniques may be useful for this purpose.
Because of its relatively short half-life, measurement of 7Be has the potential to examine
rates of short-term soil redistribution or erosion associated with a single event. The results
of this research show that 7Be is present mainly in the surface layers of the soil and can be
spectrometric techniques. The factors identified as controlling 7Be areal activity densities
will add significantly to the future development of nuclear techniques for quantitative
106