Some Additional Parameters To Estimate Domain State From Isothermal Magnetization Measurements

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Earth and Planetary Science Letters 213 (2003) 337^345


www.elsevier.com/locate/epsl

Some additional parameters to estimate domain state from


isothermal magnetization measurements
Karl Fabian 
Universita«t Bremen, FB Geowissenschaften, Postfach 330440, 28334 Bremen, Germany

Received 6 January 2003; received in revised form 26 May 2003; accepted 3 June 2003

Abstract

Domain state and mixing analysis based on isothermal magnetization measurements is often restricted to the use of
the Day plot. In order to make more information from simple rock magnetic measurements accessible for the
quantitative analysis of domain state, four additional parameters are proposed. Two of them, a hysteresis shape
parameter and a coercivity ratio, can be directly calculated from standard measurements of the hysteresis loop and
backfield curve. The other two, a transient energy dissipation ratio and the viscosity of isothermal remanent
magnetization, require additional measurements, which, however, do not increase measurement time noticeably. The
theoretical background of the above parameters is discussed. Their ability to discern domain state is shown for a small
set of synthetic magnetite and titanomagnetite samples and in a case study of a transect from the rim to the center of
a dredged mid-ocean ridge basalt.
+ 2003 Elsevier B.V. All rights reserved.

Keywords: rock magnetism; hysteresis

1. Introduction dependent measurements belong to this group.


Isothermal measurements are especially conven-
In rock and environmental magnetism isother- ient, because they can be performed fast and
mal magnetization measurements provide the easily even on large sample sets. In the following
most simple and fundamental quantities to esti- the terminology and notation of [1] are used. The
mate domain state of the remanence carriers. standard procedure to estimate domain state in
The notion of isothermal magnetization measure- rock magnetism is the Day plot [2]. It is based
ment subsumes a number of very di¡erent mea- on the measurement of two isothermal magneti-
surement procedures. All types of hysteresis mea- zation curves. The hysteresis loop consisting of an
surements, including initial curve and minor loops upper branch Mþ (B) and a lower branch M3 (B)
as well as remanence measurements and even time as well as the back¢eld curve Mbf (B). From this
large set of measurements, only four parameters
are extracted: The saturation magnetization Ms is
usually approximated by interpreting the high
* Tel.: +49-421-218-3938; Fax: +49-421-218-7008. ¢eld slope of Mþ (B) as representing the paramag-
E-mail address: karl.fabian@uni-bremen.de (K. Fabian). netic susceptibility, which then is subtracted from

0012-821X / 03 / $ ^ see front matter + 2003 Elsevier B.V. All rights reserved.
doi:10.1016/S0012-821X(03)00329-7

EPSL 6728 5-8-03


338 K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345

both hysteresis branches to obtain the ferro- or the hysteresis properties of well-de¢ned homoge-
ferrimagnetic loop. By de¢nition, Ms is the high neous materials. In applied rock magnetism, iso-
¢eld asymptotic value of the latter. A more re- thermal magnetization measurements are used as
¢ned technique to extrapolate for Ms using an diagnostic tools to interpret the properties of
approach to saturation law has been proposed complex mineral and grain-size mixtures. This re-
in [3]. The second value is the saturation rema- quires to represent the additional information by
nence Mrs de¢ned as Mþ (0). The ratio Mrs /Ms is robust quantitative parameters which have a clear
high, if the sample is not able to demagnetize physical meaning independent of very special as-
itself by the action of its self-induced magnetostatic sumptions about mineralogy and grain size. In
^ or self-demagnetizing ^ ¢eld. High Mrs /Ms is this respect, the suitability of some additional hys-
therefore indicative of single-domain (SD) or teresis parameters, partly suggested in [10], has
pseudo-single-domain (PSD) particles as rema- already been tested in [11].
nence carriers. On the other hand, low Mrs /Ms Here, another four quantitative parameters are
indicates e¡ective self-demagnetization. This oc- presented. They also are partly based on previous
curs either by formation of magnetic domains studies [1,12]. Two of them ^ the shape parameter
for large multi-domain (MD) remanence car- chys and the coercivity ratio Brh /Bcr ^ allow to
riers or by thermally activated magnetization re- extract additional information from the stan-
versal if superparamagnetic (SP) particles are dard isothermal data sets of M (B), Mbf (B).
abundant. Further, the coercive force Bc , de¢ned Their information content is not directly related
by M3 (Bc ) = 0, and the coercivity of remanence to Mrs /Ms and Bcr /Bc , although Brh /Bcr is also
Bcr , de¢ned by Mbf (Bcr ) = 0, are obtained from indicative of domain state. Moreover, two simple
the measured magnetization curves. The ratio extensions of the classical isothermal measure-
Bcr /Bc again is indicative of domain state. The ment scheme are proposed, which allow for even
theoretical value for an isotropic ensemble of uni- more detailed domain state investigation, without
axial non-interacting SD particles is 1.09 [4], for noticeably increasing experimental e¡ort or mea-
large MD magnetite, Bcr /Bc v 5. surement duration. They involve the measurement
Often, rock and environmental studies con¢ne of an additional hysteresis branch Msi (B) and the
the quantitative domain state interpretation of inclusion of an estimate of viscosity of isothermal
their isothermal measurement curves to the Day remanent magnetization (VIRM).
plot, which incorporates only the above ratios
Mrs /Ms , Bcr /Bc . Although indeed a lot of informa-
tion about domain state and mixing can be di- 2. Transient energy dissipation (TED)
rectly or indirectly inferred from the Day plot
[5,6], there still is much additional information From a physical point of view, the most easily
left in the original data set M (B), Mbf (B), which accessible parameter proposed here is TED.
can help to resolve the often remaining ambigu- The essential physical di¡erence between SD
ities in practical applications. There exist quite a and MD particles is that the self-induced magne-
number of interesting and valuable approaches to tostatic ¢eld in MD particles is su⁄cient to par-
use this remaining information. Mathematical tially demagnetize the particle by irreversible pro-
analysis of hysteresis loops allows to infer Fourier cesses such as domain wall nucleation or domain
expansions [7] or coercivity spectra [3] which con- wall pinning by inclusions or defects. Note that
tain the complete information about the loops. reversible demagnetization due to spin rotation or
Additional measurement of a dense set of ¢rst thermally activated switching ^ as in SP particles
order reversal curves yields a two-dimensional ^ occurs also in SD ensembles and is responsible
picture of a special switching ¢eld distribution for ambiguity in Mrs /Ms .
of the sample [8,9]. There exists extensive litera- The slightly extended hysteresis measurement
ture about hysteresis modelling in the material scheme proposed in [1] and shown in Fig. 1 allows
sciences, but their aim is to understand and model to determine exactly the energy which is dissi-

EPSL 6728 5-8-03


K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345 339

+
M (B)
sotropy, exchange energy and magnetostriction.

Increasing the ¢eld back to Bmax along the mag-
Mrs Msi(B) M (B) netization curve Msi (B) reverses the above pro-
cesses. Yet, in PSD and MD remanence carriers
-Brh wall pinning and nucleation failure lead to a gap
M
Bc Bcr between Mþ (B) and Msi (B). The area Evt of this


E t/2
gap is equivalent to half the TED initiated solely
M (B)+Mrs by the action of the self-demagnetizing ¢eld. The
Ehys
factor 2 in Eq. 1 takes into account the symmetric
processes for negative ¢eld values.
The ratio between Evt and the total hysteresis
B
area:
Fig. 1. Extended hysteresis measurement including determina- Z Bmax
tion of the Msi curve. The dark shaded area corresponds to E hys ¼ ðM þ ðBÞ3M 3 ðBÞÞdB ð2Þ
half of Evt . The other half is contained in the symmetric 3Bmax
curve at negative ¢elds. The total area between the lower
hysteresis branch M3 (B) and the upper branch Mþ (B) is de- determines which fraction of the total energy dis-
noted by Ehys . Also indicated are the de¢nitions of Mrs , Bc , sipation is related to TED. In ideal non-interact-
Bcr and Brh . ing SP^SD mixtures Evt = 0 since in both constit-
uents no irreversible processes are induced by the
pated by the above irreversible self-demagnetiza- self-demagnetizing ¢eld. As long as Ehys g0, also
tion processes. The measurement is performed in the ratio Evt /Ehys is zero for these mixtures. Due to
the following way: magnetostatic interaction Evt /Ehys in real SP^SD
ensembles deviates from zero. However, samples
1. Apply B = Bmax and then set B = 0 to prepare with Evt /Ehys 6 5% can safely be interpreted as
the sample in the state of saturation remanence interacting SP^SD mixtures. In MD samples
Mrs . In order to avoid overshooting to negative Evt /Ehys can rise above 50% as shown in Fig. 2.
¢elds in our alternating gradient ¢eld magneto- The most important property of Evt /Ehys is that
meter it turned out to be useful to reset the it varies continuously with grain size over the
¢eld to zero in two or three steps (10, 1 and whole SD^MD spectrum. Most notably, it is not
0 mT). in£uenced by SP grain-size fractions, since no ir-
2. Measure initial curve plus hysteresis loop start- reversible processes occur in SP particles. In this
ing from this state. The thus obtained ’initial respect, the TED ratio Evt /Ehys is less ambiguous
curve’ is the saturation initial curve Msi (B) [1]. than Mrs /Ms , which cannot discriminate between
reversible and irreversible self-demagnetization.
The energy: Therefore, Mrs /Ms decreases with increasing grain
Z Bmax size, but also with increasing SP content. Of
E vt ¼ 2 ðM þ ðBÞ3M si ðBÞÞdB ð1Þ course, as with Mrs /Ms , it is neither possible to
0
discriminate mixtures of SD and MD particles
is dissipated solely by transient irreversible pro- from PSD particles by Evt /Ehys , nor is it possible
cesses initiated by the action of the self-demagnet- to distinguish chemical alteration and changes of
izing ¢eld of the sample. In a su⁄ciently high internal stress from grain-size variation. Yet, it is
maximal ¢eld Bmax all magnetic spins are nearly a most reasonable parameter for average ‘mag-
aligned with the ¢eld. Only reversible rotations or netic grain size’.
para-processes occur at high ¢elds. Reducing the
¢eld to B = 0 along the magnetization curve
Mþ (B) results in domain nucleation and wall 3. A coercivity ratio related to TED
movement if the self-demagnetizing ¢eld is strong
enough in comparison to magnetocrystalline ani- It is possible to derive coercivity related ratios

EPSL 6728 5-8-03


340 K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345

0 0.1 0.2 0.3 0.4 0.5 0.6 0.7

2.6 2.6

A14
2.4 ~1.91 µm 2.4

2.2 A18 2.2


W6 ~0.58 µm
~12.1 µm
2 2
W5
~8.3 µm

1.8 A15 1.8

Brh / Bcr
~0.74 µm
W4
~5.7 µm
1.6 1.6

W1 A17
1.4 1.4
~0.7 µm ~0.18 µm
A21
1.2 ~0.09 µm 1.2
W2
W3 ~0.5 µm
~0.5 µm
1 1

0.8 0.8

0 0.1 0.2 0.3 0.4 0.5 0.6 0.7



E t / Ehys

Fig. 2. The ratio Brh /Bcr in dependence on TED Evt /Ehys


for synthetic magnetite and titanomagnetite samples. The magnetite sam-
ples W1^W6 are produced by Wright Industries and described in [13]. The titanomagnetite samples A14, A15, A17, A18 and
A21 are described in [14]. The linear relationship between the two ratios shows that Brh /Bcr is well suited as a domain state indi-
cator.

which also re£ect TED [1]. Especially the ratio 6. This indicates that mixtures containing both SP
Brh /Bcr is useful in this respect since it can be and SD particles are not well described by a stable
determined from standard magnetization mea- positive Preisach function. A possible explanation
surements M (B), Mbf (B). By de¢nition [10,3], is predominant negative interaction e¡ects be-
Brh is the median destructive ¢eld of the vertical tween stable SD and SP particles. Yet, the above
hysteresis di¡erence : behavior of Brh /Bcr is extremely useful for domain
M þ ðBÞ3M 3 ðBÞ state analysis, since it clearly separates SP, SD
M rh ðBÞ ¼ ð3Þ and MD domain states by a single easily deter-
2
mined parameter. The linear relationship between
In [11] it has been denoted by MDFhys . Graphi- Brh /Bcr and Evt /Ehys in Fig. 2 provides evidence
cally, Brh is the positive ¢eld value where the dif- that Brh /Bcr indeed is indicative of domain state.
ference between upper and lower hysteresis Yet, it must be emphasized that Evt /Ehys has a
branches has decreased from 2Mrs at B = 0 to direct physical meaning which shows that it is
Mrs or where the upper hysteresis branch inter- linked to domain state, whereas Brh /Bcr is an in-
sects with the lower branch after shifting the latter ferred quantity, the physical interpretation of
upward by Mrs . It has been shown in [1] that which is not equally clear. Brh /Bcr can serve as a
for samples with stable positive Preisach function substitute for Evt /Ehys for the extended interpreta-
Brh /Bcr v 1, and that an approximative calculation tion of already existing hysteresis loops. However,
yields: it is recommended to rely on Evt /Ehys when the
M þ ðBrh Þ3M si ðBrh Þ necessary measurement of Msi (B) is possible.
Brh =Bcr W1 þ ð4Þ
M rs
This estimate relates Brh /Bcr to the gap between 4. Quantifying hysteresis shape
Mþ (B) and Msi (B) and consequently to the ratio
Evt /Ehys . Thus, high Brh /Bcr ratios indicate preva- Shape anomalies of hysteresis loops are fre-
lence of transient irreversible processes and there- quently interpreted as being indicative of SP par-
fore large particles. On the other hand, in natural ticles [15] or more generally for mixtures of frac-
ensembles containing SP particles Brh /Bcr ratios tions with highly contrasting coercivities [16,17].
below 1 are observed as will be seen in Section There are few attempts to quantitatively use hys-

EPSL 6728 5-8-03


K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345 341

2 Bc lied’ to ‘wasp-waisted’ loops. Since calculation


of chys requires only the standard hysteresis loop
a) 2 MS M (B), it can be easily included in rock and en-
vironmental magnetic studies.
In Fig. 4 measurements of chys for a small se-
lection of sized magnetite and titanomagnetite
b) samples are shown. They indicate that chys is rel-
atively independent of grain size within the SD^
MD region. This is important because variations
in chys are indicative of either admixture of SP
c) particles or for the presence of an independent
mineral fraction.
Fig. 3. A simple way to quantify the shape of a hysteresis
loop is to compare the area Ehys with an ideal rectangular
area. A hypothetical ideal loop (B) consists of two congruent
branches which cross the B axis at 3Bc and +Bc , respec- 5. VIRM
tively. The horizontal distance between the branches at each
magnetization is 2Bc , thus the total area is 2Bc U2Ms . In VIRM is measured by monitoring the decay of
case of a ‘wasp-waisted’ loop (a), the area Ehys is larger than an IRM acquired in some high ¢eld Bmax [20,12].
4Ms Bc , whereas for ‘potbellied’ loops (c) Ehys 6 4Ms Bc . The
The temporal evolution of the magnetization is in
areas on the right show symmetric plots of the horizontal
width B(M) obtained by subtracting the hysteresis branches good approximation given by:
horizontally. MðtÞ ¼ M 0 3S logðt=t0 Þ ð6Þ
Measurement of M(t) over some reasonable time
teresis shape information. The ww factor of interval allows to determine the normalized value
[18,19] allows to assess the constriction of the S/M0 which is indicative of the presence of mag-
hysteresis loop, but cannot discriminate among netizations with relaxation times near t0 . This is
non-constricted (‘potbellied’) loops, which all related to the frequency dependence of suscepti-
have ww = 1. Consequently, only very inhomoge- bility in the vicinity of the frequency 1/t0 . High
neous mixtures with large content of both constit- S/M0 is indicative of grain sizes close to the tran-
uents are detectable and ww varies extremely non- sition from SP to stable SD grains. Usually a 100 s
linearly with mixing ratio. Here the following
0 0.1 0.2 0.3 0.4 0.5 0.6
more linearly behaving and more sensitive shape 1 1

parameter chys is advertised. It is de¢ned by: 0.8 0.8

 
E hys 0.6 0.6

c hys ¼ log
4M s Bc
ð5Þ 0.4 SP 0.4

0.2 0.2

where log represents the natural logarithm. The


hys

0 0

shape parameter chys compares the actual area -0.2 -0.2

Ehys of the hysteresis loop with the rectangular -0.4 -0.4

SD MD
A14 TM60
area with height 2Ms and width 2Bc . The latter -0.6
W3
W1
~0.7 m
A17 TM60 W4
W6
~12.1 m ~1.91 m
-0.6
~0.18 m ~5.7 m
area corresponds to an ‘ideal’ hysteresis loop hav- -0.8
~0.5 m

W2
A21 TM60
W5
~8.3 m
A18 TM60
~0.58 m A15 TM60
~0.74 m
-0.8
~0.5 m

ing two congruent branches, one passing through -1


~0.09 m

-1

zero at 3Bc , the other at +Bc . As shown in Fig. 3, 0 0.1 0.2 0.3
E ∆
/ Ehys
0.4 0.5 0.6

t
for wasp-waisted loops Ehys s 4Ms Bc and accord-
ingly chys s 0, whereas for potbellied loops Fig. 4. Measurement results for a suite of synthetic (titano)-
magnetite samples. Independent of grain size and composi-
Ehys 6 4Ms Bc and chys 6 0. The logarithmic de¢- tion, all synthetic samples show chys values in the range
nition of chys is intended to obtain a relatively from 30.9 to 30.5. Evt /Ehys varies continuously with grain
linear measure of shape variation from ‘potbel- size, but apparently is increased by magnetostatic interaction.

EPSL 6728 5-8-03


342 K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345

Fig. 5. Cross-section of hysteresis parameters along a zero age MOR basalt T787-R1 (sample provided by D. Kent). Sample posi-
tion varies only approximately linearly with distance from the chilled margin. The total length of the MORB specimen is 12 cm.
As shown by Gee and Kent [19], the grain size increases steadily from SP^SD mixtures at the chilled margin to PSD^MD par-
ticles. Mas denotes the ‘apparent’ saturation magnetization as obtained by subtracting the average slope of the hysteresis loop
above 70% of the maximum ¢eld (here 1 T).

VIRM measurement can be easily included into a particles. Of course, the best solution is to set
hysteresis measurement scheme. Experimental ex- up more reliable special equipment for this mea-
perience, however, shows that VIRM measure- surement as suggested in [12].
ments, e.g. using the ‘magnetization versus time’
option of the MicroMag (Princeton Measurement
Inc.), often result in very noisy data, since the 6. A case study of a transect along a mid-ocean
signal is very small and any vibrations due to ridge basalt (MORB)
air movement or other external in£uences induce
spurious oscillations in the magnetization curve. As convincingly demonstrated in [19], there is a
Such oscillations must be discarded and often systematic variation in domain state from SP over
only the ¢rst few measurement points can be SD to PSD/MD along a 12 cm transect from the
used to estimate S/M0 and large error margins chilled outer margin of a MORB to its center.
have to be taken into account. Still it is recom- Here a densely sampled zero age MORB (sample
mended to add this simple measurement to the T787-R1 provided by D. Kent) is used as a case
standard laboratory routine, because noisy data study in order to test this conclusion on the basis
are better than no data and increased viscosity of the parameters proposed above. Already the
is a valuable indication for the presence of SP data in Fig. 5 show that the SD^MD trend is

EPSL 6728 5-8-03


K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345 343

0 0.05 0.1 0.15 0.2 0.25 0.7 0.8 0.9 1 1.1 1.2 1.3 1.4

1 1 1 1

1.2
0.8 0.8

SP
0.6 1.1 0.6
0.5 0.5

Brh/Bcr
0.4 1 0.4

0.2 0.2
0.9
σ hys

0 0

σ hys
0 0
0.8
-0.2 0 0.05 0.1 0.15 0.2 0.25 -0.2
E∆t/Ehys

SD MD
-0.5 -0.5 -0.4 -0.4

-0.6 -0.6

-0.8 -0.8
-1 -1

0 0.05 0.1 0.15 0.2 0.25 -1 -1


E∆t / Ehys
0.7 0.8 0.9 1 1.1 1.2 1.3 1.4
Brh/Bcr
Fig. 6. Plot of chys versus Evt /Ehys for the hysteresis data of
the MORB sample T787-R1. Fig. 7. Plot of the shape parameter chys versus Brh /Bcr for
the hysteresis data of the MORB sample T787-R1. The inset
shows that Brh /Bcr varies monotonously with Evt /Ehys in the
unambiguously represented by Evt /Ehys . Note that SD^MD transition region.
this parameter is not in£uenced by SP fractions.
Grain-size variation within the SP^SD transition
region is resolved by S/M0 . The anomalous region viscous IRM versus Evt /Ehys in Fig. 8 traces the
between position 28 and 41 is due to an increase presence of low energy barriers in dependence on
of e¡ective grain size, not due to SP admixture. the presence of transient irreversible processes. In
Otherwise Evt /Ehys would not be in£uenced. the SD region, viscous processes due to low en-
In Fig. 6 shape parameter chys is plotted versus ergy barriers are the hallmark of an SP fraction.
Evt /Ehys , which yields an extremely clear picture of Interestingly, there also is a slight but signi¢cant
the grain-size variation. Over the whole SD^PSD increase of S/M0 with grain size. This indicates
range, chys varies only slightly around 30.5, that viscous processes in MD grains cannot be
whereas SP-in£uenced samples have chys values completely discarded. This result agrees with the
above 30.2. The lowest chys values occur in the ¢nding of [21] for sized magnetite, but di¡ers
anomalous region of positions 28 through 41. from the conclusion of [12]. Comparison with
This again discards the possibility of SP admix- Fig. 5 shows that especially samples from the
ture which should have increased chys . The de- anomalous region of positions 28^41 have high
creased values of about 30.7 are closer to the viscosity values comparable to those in the SP^
values from the synthetic titanomagnetites of SD transition region. On its own, viscous IRM as
Fig. 4 and therefore rather indicate stress release 0 0.05 0.1 0.15 0.2 0.25

in the anomalous region. Alternatively, chys may 2500 2500

re£ect a variation of the oxidation state within the


anomalous region and across the transect. 2000 2000

When only data from the standard isothermal SP


measurement M (B), Mbf (B) are used, it is still 1500 1500
S/M0 [ppm]

possible to plot chys versus Brh /Bcr as in Fig. 7.


1000 1000
Here the SP^SD variation is especially clearly re-
solved, since not only chys increases, but also
MD
500 500
Brh /Bcr adopts values 6 1 within this region.
Although the SD^PSD transition appears to be SD
0 0
less clearly resolved, the variation of Brh /Bcr 0 0.05 0.1 0.15 0.2 0.25

closely mirrors the variation of Evt /Ehys as is E t / Ehys

shown in the inset of Fig. 7. Fig. 8. Viscous IRM versus Ev t/Em hys for MORB sample
According to its physical meaning, the plot of T787-R1.

EPSL 6728 5-8-03


344 K. Fabian / Earth and Planetary Science Letters 213 (2003) 337^345

an SP indicator therefore appears to be more am- References


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Acknowledgements [13] D. Kra¤sa, R. Leonhardt, N. Petersen, Experimental pro-
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