7030 Counting Instruments

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7030

Counting Instruments
Approved by Standard Methods Committee, 2011. Editorial revisions, 2020. Joint Task Group: 22nd Edition—Robert T. Shannon.

7030 A. Introduction

Radiochemical analytical instruments operate on the princi- instruments may also be used for analysis. Instrument back-
ple that the energy expended by a radiation event is detected ground and fractional counting efficiency must be measured
and recorded by an instrument suitable for the type of radiation and integrated into the sample calculations. These characteris-
emitted. The counting instruments described below are com- tics can be compared with historical data and used to evaluate
monly found in radioanalytical laboratories. Other less common instrument stability.

7030 B. Description and Operation of Instruments

1. Gas-Flow Proportional Counters counting gas. With thin-window GPCs, the test source is positioned
outside the active volume of the detector, next to an entrance win-
Gas-flow proportional counters (GPCs) detect and quantify dow generally constructed of a very thin Mylar film. The entrance
alpha- and beta-emitting radionuclides. If the sample contains window allows decay particles emitted from the source to enter
multiple radionuclides, the instrument will detect and count all the active volume of the detector.
emissions regardless of their radionuclide source or energy. The Thin-windowed GPCs are less sensitive to low-energy decay
analysis may be made radionuclide-specific by combining this particles than internal GPCs due to the less favorable counting
detection method with a radiochemical separation to segregate geometry associated with positioning the source outside the active
the desired radionuclide. The radionuclide (226Ra, Th, U, etc.) is volume of the detector. Additionally, there are losses due to the
usually precipitated and mounted as a thin layer (generally less decay particles’ interaction with air and the window between the
than 5 mg/cm2) on planchets. test source and the active volume. In contrast, windowed GPCs
a. Types of GPCs commonly used for environmental analyses: are much less subject to counting-chamber contamination and
GPCs operate on the principle that radioactive decay particles, damage due to loose residues, losses due to residual moisture, and
such as alpha and beta particles, cause ionization in a gas-filled corrosion due to vapors commonly associated with test sources.
detector. The liberated electrons are accelerated in an electrical Prepare all GPC test sources in a manner that minimizes friable
field placed across the detector cell, thereby amplifying the signal. particles and vapors from moisture or solvents because these can
The signal is collected at the detector’s anode, creating a pulse of contaminate or damage the detector chamber (internal GPCs) or
electricity that then can be processed. The combined magnitude detector entrance window (thin-windowed GPCs).
of all pulses collected from one decay particle is proportional to c. Detection system components: The instrument consists of a
the energy deposited in the detector by that particle—hence the counting chamber, pre-amplifier, amplifier, scaler, high-voltage
term proportional count. power supply, timer, pulse-shape discriminator, and register. Use
Select the detector fill gas to optimize amplification. Although the specified counting gas and accessories, make adjustments for
other gases have been used successfully, the most frequently used sensitivity, and operate in accordance with both the method and
mixture in low-background GPCs is called P-10; it consists of the manufacturer’s instructions.
90% argon and 10% methane. d. Background-reduction measures: Low backgrounds are
Alpha particles may be determined by operating the detector at important for environmental analysis. One technique for minimiz-
the alpha plateau, where the voltage is low enough that the detector ing background activity is constructing the detection system with
does not respond to beta particles. Detectors are frequently oper- low-background materials. Two other techniques used for back-
ated at the higher-voltage beta plateau, where the detector responds ground reduction—passive and active shielding—are designed to
to both alpha and beta particles. Because each pulse produced is minimize the effect of external radiation (e.g., cosmic radiation as
proportional to the energy deposited in the active volume of the well as gamma and X-ray radiation from terrestrial sources, build-
detector by the decay particle, pulse-height analysis (PHA) can ing materials, and radioactive sources at the laboratory). A passive
be used to discriminate between the larger pulses associated with shield typically consists of a 5- to 10-cm-thick layer of lead sur-
alpha particles and the smaller pulses associated with beta particles. rounding the detector. An active shield involves a guard detector
b. Internal and thin-windowed GPCs: Internal and thin-win- placed next to the primary detector so any radiation that impinges
dowed GPCs are commonly used for low-level environmental on the primary detector must pass through the guard detector. The
measurements. With internal GPCs, the test source is introduced primary detector is operated in anticoincidence mode (i.e., any
directly into the counting chamber, which is then filled with the counts registered concurrently in the primary and guard detectors

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7030 COUNTING INSTRUMENTS - B. Description and Operation of Instruments

Figure 7030:1. Shape of counting rate-anode voltage curves. Key: (a) and (b) are for internal proportional counter with P-10 gas; (c) is for end-window
Geiger-Mueller counter with Geiger gas (Note: Beta losses depend on radiation energy and thickness of window and air path.)

are not registered as valid sample counts). With these measures, varies by less than 5% per 100-V change in voltage. Distributed
modern low-background GPCs can routinely achieve background planar test sources are the most common test source counted in
count rates on the order of 0.05 to 0.2 alpha counts per minute most laboratories. When plateaus are obtained using distributed
(cpm) and 0.5 to 2 beta cpm. sources, the slope of the curve at the operating voltage may nomi-
e. Availability: GPC detection systems are commercially avail- nally exceed a target of 5% per 100 V. Check the plateau to ensure
able in a number of assembled configurations. Detectors may that the optimal operating voltage has not changed by performing
be configured alone or in arrays (e.g., of 4, 8, and 10 detectors), instrument response and background checks after each change of
and may incorporate automatic sample changers. The most com- counting gas.
monly encountered detector diameter is approximately 5 cm. Ten- Most modern GPC software contains utilities for perform-
centimeter detectors are also available; they are most frequently ing plateau curve acquisition and establishing operating
used to count larger sources (e.g., air filters). voltage set-points. Consult the instrument manual for setup
f. Instrument setup: details.
1) Radioactive sources—See Section 7020 A.3h. 3) Pulse-height discriminator setup—GPCs use pulse-height
2) Voltage plateau (alpha or beta)—A voltage plateau is a analysis (PHA) to discriminate between pulses originating from
curve used to determine an operating voltage that will provide alpha or beta particles based on the amplitude of the pulses they
reproducible count rates. It is obtained by placing an appropriate produce. Due to the physics of the measurement, alpha pulses
alpha or beta source in each detector and varying the detector are generally much larger than beta pulses. Crosstalk refers to
voltage until the change in the count rate reaches a minimum. the unavoidable misclassification of pulses during simultaneous
Further increases in voltage will produce little change in overall counting for alpha and beta. For example, pulses resulting from
detector response until the plateau region is exceeded. Caution: alpha decays may be misidentified as beta pulses (alpha-to-beta
Continuous discharge at too high a voltage will damage the crosstalk), or pulses resulting from beta decays may be misidenti-
instrument. fied as alpha pulses (beta-to-alpha crosstalk). Alpha particles are
The alpha plateau is generally a region in the 300 to 800 V much more strongly attenuated than beta particles, so they often
range (depending on the detector) where the instrument responds result in smaller pulses that may be misclassified as beta pulses.
to an alpha source but not a beta source. The beta plateau is gen- In other words, alpha-to-beta crosstalk will be much larger than
erally a region in the 1000 to 1700 V range where the instrument beta-to-alpha crosstalk.
responds to both alpha and beta radiation. Setting the pulse-height discriminator establishes the instru-
The relative counting rate (ordinate) is plotted against the volt- ment’s crosstalk response. Some instruments require that discrim-
age (abscissa). The operating point is generally established on the inators be set up after the operating voltage is established, while
plateau curve at a point marginally beyond the knee of the curve others are configured at the factory. Consult the instrument manual
(Figure 7030:1), where instrument response to a point source for setup details. As an overall measurement strategy, setting the

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7030 COUNTING INSTRUMENTS - B. Description and Operation of Instruments

discriminators to minimize beta-to-alpha crosstalk (e.g., to ~0.1%) 7) Sample counting—Place the prepared sample test source
will decrease the magnitude of crosstalk corrections and improve in the detector in a geometry consistent with initial calibration.
the quality of simultaneous alpha and beta measurements. For internal GPCs, ensure that there is electrical contact between
Once the operating voltage and discriminator settings have planchet and chamber, and flush the chamber with counting gas.
been established, they must be documented and locked down. Count for a preset duration or a preset count to give the desired
Changing either parameter invalidates all previously established counting uncertainty (Section 7020 D).
performance check data and instrument calibrations, and the
instrument must be recalibrated. 2. Alpha Scintillation Counter
4) Background (alpha or beta)—Most detectors have a back-
ground count rate that is due to several factors: cosmic radiation; Alpha scintillation counters detect and quantify alpha-emitting
radionuclides contained in instrument materials; the counting radionuclides. If the sample contains multiple radionuclides, the
room’s construction material; undesirable signals from electron- instrument will detect and count all alpha emissions regardless of
ics; and the proximity of radioactive sources. The background is their radionuclide source or energy. The analysis may be made
roughly proportional to the size or mass of the counting chamber more radionuclide-specific by using a radiochemical separation
or detector but can be reduced by shielding or anti-coincidence to isolate the desired radionuclide. This radionuclide (226Ra,
guard circuitry (see ¶ d above). Th, U, etc.) is usually precipitated and mounted as a thin layer
a) Determination of background count rate—The background (≤5 mg/cm2) on planchets. Radon-222 (radium-226 by radon
count rate is subtracted from each measurement to determine the emanation) also can be counted in alpha scintillation cells in a
net activity of the sample test source. Determine the background modified sample chamber (Section 7500-Ra C).
count rate by counting an empty planchet in the counting chamber a. Principle and uses: An alpha particle interacts with zinc
in the same configuration as the sample test source. The back- sulfide phosphor (which contains a silver activator), exciting the
ground count duration should be as long as or longer than the scintillator’s atoms. When the atoms return to the ground state,
counts from which it will be subtracted. they emit the energy as visible light. This process is called scin-
b) Control of backgrounds—Verify the continuing stability tillation. The light is further transformed into an electrical current
of the background count rate during the count by tracking back- via an attached PMT, which amplifies the electrical current into a
ground performance via control charts. Also, evaluate method measurable pulse. The pulses trigger a scaler, which counts each
blank control charts for persistent high or low bias in results (i.e., pulse. Depending on the amount of radionuclide present and sta-
absolute bias), then determine the cause and correct it. If the cause tistics required, count a sample long enough to obtain required
is intrinsic to the method, a correction factor (independent of QC sensitivity. The counter is calibrated with a thin-layered precipi-
samples) may be developed and applied to eliminate absolute bias tate of a radionuclide or an electrodeposited radionuclide.
as long as the additional correction’s uncertainty is reflected in b. Components: The alpha scintillation counter consists of a light-
the combined standard uncertainty reported for the sample result. tight sample chamber with a phosphor detector coupled to a photo-
5) Initial calibration (alpha, beta, or radionuclide specific)— multiplier tube (PMT) and sample holder, a high-voltage supply, an
The purpose of initial calibration is to empirically derive counting amplifier-discriminator, a scaler, and readout capability. Generally,
efficiency factors for a geometry that matches those of the test the PMT’s window has a larger diameter than that of the samples.
samples, thus ensuring that the correction for efficiency is accu- Put the phosphor between the sample and the PMT. The distance
rate. Parameters that must match include radionuclide, matrix between the sample surface and PMT face is usually about 3 to
composition, and density and thickness (which causes self-ab- 5 mm. Arrange the phosphor so the PMT window is in optical con-
sorption of alpha or beta particles in the sample matrix). Each tact with the scintillator. Under these conditions, the counting effi-
detector’s detection efficiency must be determined separately. Ini- ciency can be 35% to 40%. For details on operating and calibrating
tial calibration is procedure dependent; see individual procedures an alpha scintillation counter, see manufacturer’s instructions.
for specific instructions. Absorption curve values do not need to c. Performance verification:
be re-established after initial calibration as long as the continuing 1) Radioactive source—See Section 7020 A.3h.
calibration (source check) response is monitored regularly and 2) Plateau—In accordance with manufacturer recommen-
indicates that the instrument has remained stable between calibra- dations, use a radioactive source to find the operating voltage
tion and sample measurements. where the count rate is consistent over some specified voltage
6) Continuing calibration (source check)—Verify instrument range.
stability at the operating voltage by counting separate check 3) Background—Two backgrounds are evaluated with alpha
sources for alpha and beta (where applicable) on each detector. scintillation counters: electronic instrument background and
Monitor the major and minor channel count rates (i.e., for an chamber background. The electronic instrument background char-
alpha source, alpha is the major channel and beta is the minor acteristically measures the PMT’s electronic noise. It is determined
channel) for each source counted and plot the results on a con- periodically (e.g., annually) by counting with an empty chamber
trol or tolerance chart to demonstrate the continuing stability of and should vary from 0 to 1 cpm.
the detector efficiency and crosstalk (Section 7020 A). The tests The chamber background is counted with the zinc sulfide phos-
and acceptance criteria used should be addressed in the laboratory phor or scintillation cell in place. This background may be caused
quality manual. If the checks do not provide evidence of continu- by a number of factors including contaminated instrument parts,
ing instrument stability, the detector should be taken offline until counting-room construction materials, and nearby sources of
the problem is fixed and the instrument is recalibrated, or until radioactivity. When measuring chamber background, use a dura-
continuing checks demonstrate that maintenance has not changed tion as long or longer than the longest sample counting duration;
instrument response. this background is subtracted from gross sample results.

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7030 COUNTING INSTRUMENTS - B. Description and Operation of Instruments

4) Initial calibration—The purpose of initial calibration is to and 14C). Counting efficiencies approaching 100% can be obtained
determine the scintillation counting efficiency based on sam- from alpha- and higher-energy beta-emitting radionuclides.
ple thickness (which causes absorption of some alpha or beta b. Components: The system consists of a liquid scintillator
particles in the sample matrix) or cell geometry (in the case of [organic scintillator(s) diluted with an appropriate solvent], a
scintillation cells). Initial calibration is method-dependent; see polyethylene or glass vial, a liquid scintillation counter (with one
individual methods for specific instructions. or more PMTs coupled to a single- or multichannel analyzer), and
Absorption curve values do not need to be re-established after a readout device.
initial calibration as long as the check source response is mon- c. Performance verification:
itored regularly and control charts indicate instrument stability. 1) Radioactive sources—See Section 7020 A.3h.
Recalibrate scintillation cells periodically. 2) Background—Consider 3 backgrounds when dealing with
5) Continuing calibration (source check)—See 7030 B.1f 6. liquid scintillation spectrometers: electronic or instrument back-
6) Sample counting—Place the prepared sample in the count- ground, chamber background, and background for subtraction.
ing chamber according to manufacturer’s instructions. Take the a) Electronic or instrument background—Periodically deter-
following precautions: mine background using an empty counting chamber and a dark
• ensure that the counting chamber is light-tight; vial. Some manufacturers supply a dark or black vial [a counting
• ensure that PMT is not exposed to direct light while high vial filled with black material (e.g., graphite)] for this purpose.
voltage is applied; b) Chamber background—The unquenched background is
• let sample chamber adapt to the dark before starting count; determined using a vial supplied by the manufacturer. This back-
• count for a preset duration or count, to give the desired ground is used only to assess daily instrument performance and
counting precision; should never be subtracted from sample results.
• ensure that the sample is in contact with the phosphor; and c) Background for subtraction—A method-specific back-
• count samples in a geometry consistent with the initial ground is determined and subtracted from each sample test
calibration. source result using vials identical to those used for samples,
except that they are free of activity. The background subtraction
sample is not a QC sample, but is part of the analytical process
3. Liquid Scintillation Counters
and should be prepared independently of QC reagent or method
blanks. When analyzing tritium, for example, mix the same type
A liquid scintillation spectrometer system uses one or more of vial with cocktail from the same production lot, using the
PMTs to count the number of scintillations (photons of light) same sample-to-cocktail ratio with an aliquant of purified dead
emitted from a sample vial. The number of photons produced water (e.g., a fossil source of water in which tritium has already
in the scintillator is proportional to the particle’s initial energy. decayed).
This information helps determine the specific radionuclide 3) Initial calibration—Before sample analysis, the counting
present. conditions may be optimized for measurements with constant
a. Principle and uses: A sample containing beta- (or alpha-) quench. For variable-quench measurements, counting regions
emitting radionuclides is mixed in a liquid scintillator. Each beta may be optimized if they take into account variation in the region
(or alpha) particle transfers kinetic energy to solvent and phos- of interest as a function of quench. Some analysts maximize the
phor molecules in the liquid scintillation cocktail via a large num- figure of merit (FOM):
ber of collisions. As the excited molecules return to ground state,
they emit photons of light that are detected by PMTs in the instru- E2/B
ment. Although the number of photons produced for any given
decay event is proportional to the energy of the decay particle, it where:
is notable that alpha particles transfer energy at roughly one-tenth
E = efficiency and
the rate of beta particles and thus result in lower energy pulses.
B = background count rate.
The PMTs amplify the incoming light into an electronic pulse. In
most instruments currently in use at radiochemistry laboratories, Optimum counting conditions should not be re-established
background is significantly reduced by operating two PMTs in after initial calibration because changing the analysis window will
coincidence. This means that signal must be received from both affect the efficiency that is determined. Once optimum conditions
PMTs within the same time interval (e.g., within 20 ns of each have been selected (via a pure source), determine sample counting
other) to yield a valid pulse. Coincident signals are summed, dig- efficiency by one of several methods (see Sections 7500-3H and
itized according to their pulse-height and then stored in a multi- 7500-Rn): standard additions, quench curve, or prepared labora-
channel analyzer in a channel corresponding to the energy of the tory standard.
original radiation. 4) Continuing calibration (source check)—See Section 7500-
Although the instrument outputs spectrometric data, the con- Rn for specific calibration procedures for radon-222 by liquid
tinuous nature of beta spectra combined with the instrument’s scintillation counting.
limited resolution limits the instrument’s use for spectrometric 5) Sample counting—Place prepared samples in the counting
determinations. Most frequently, LS counting is combined with chamber, let samples adapt to the dark, and count for the preset
chemical separations to perform sensitive, radionuclide-specific count or duration needed to obtain the desired sensitivity.
determinations of alpha and beta emitters. Liquid scintillation is As with other counting techniques, deal with any interferences to
commonly used to determine the activities of some alpha (e.g., the method. Such interferences include quenching (chemical, color,
222
Rn and daughters) and most low-energy beta emitters (e.g., 3H or particle quenching), chemiluminescence, photoluminescence,

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7030 COUNTING INSTRUMENTS - B. Description and Operation of Instruments

static electricity, scintillation volume variations, sample homoge- 5. Gamma Spectrometers


neity, background, multiple radionuclides, and phase separation.
Gamma spectrometry identifies and quantifies specific energy
4. Alpha Spectrometers photons (gamma rays), quantitating specific radionuclides.
a. Principle and uses: Gamma rays from a sample enter the
a. Principle and uses: An alpha spectrometer detects, identi- sensitive volume of the detector and cause ionization. The lib-
fies, and quantifies specific alpha-emitting radionuclides. The erated charge is converted into a voltage pulse whose ampli-
radionuclides should be chemically separated from samples and tude is proportional to the photon energy. Pulses are stored in
deposited as a thin layer on filter papers or electrodeposited on sequence in finite energy-equivalent increments over the desired
metal disks. When a sample’s alpha emissions cause ionization spectrum. After sample counting, the accumulated pulses over
in a solid-state detector, a pulse of current is produced that has an a certain area result in photopeaks that can be identified and
amplitude proportional to the alpha particle energy. attributed to specific radionuclides based on their characteristic
The current is collected, amplified, sorted according to depos- energies.
ited alpha energy, and displayed on a multichannel analyzer. b. Components: A gamma spectrometer consists of a detector,
Chemical yield tracers should be added to each sample to ensure pre-amplifier and detector bias supply, pulse-height analyzer sys-
accurate quantitation. tem, data readout capability, and shielded sample enclosure. The
b. Components: An alpha spectrometer consists of a sample pulse-height analyzer system consists of a linear amplifier, an
chamber (with detector, sample support, and vacuum chamber); a analog-to-digital converter (ADC), memory storage, and a logic
mechanical vacuum pump; detector bias voltage supply; pream- control mechanism. The logic-control capabilities allow data stor-
plifier; amplifier; multichannel analyzer (with ADC and memory age in various modes and data display or recall. For details on
storage); and data readout capability. For details on calibration and operating and calibrating a gamma spectrum analyzer, see manu-
operations, see the operations manual provided by the manufacturer. facturer’s instructions.
c. Performance verification: Commonly used gamma detectors consist of intrinsic or
1) Radioactive source—See Section 7020 A.3h. high-purity germanium (HPGe). Lithium drifted germanium
2) Detector voltage—Set detector operating voltage in accor- [Ge(Li)] detectors are less robust, and many have been replaced
dance with the manufacturer’s recommendations. by HPGe detectors. Sodium iodide [NaI(Tl)] and silicon [Si(Li)]
3) Background—Determine the chamber background count detectors are sometimes encountered, but have limited application
using a clean filter or metal disk identical to those on which sam- (primarily to screen samples or analyze single gamma-emitting
ples are mounted. The counting duration should be at least as long radionuclides). Germanium detectors offer excellent resolution
as the longest sample counting duration. Monitor the background and reasonable to good efficiency (depending on the application
count rate (which is subtracted from the sample count rate) via a and cost). NaI(Tl) detectors have poor resolution and reasonable
control chart to demonstrate its stability over the most recent 3 to good efficiency at reasonable cost. Si(Li) detectors have good
to 10 counts and to identify potential long-term trends that could efficiency and reasonable resolution for low-energy X-rays (10
prevent the detector from providing results that meet detection to 200 KeV). Other detectors are available. See Table 7030:1 for
limit requirements. typical resolution for several detector types.
4) Initial calibration—The purpose of initial calibration is to c. Performance verification:
establish a detector’s energy calibration and counting efficiency. 1) Radioactive sources—See Section 7020 A.3h.
Use a standard source, as described in Section 7020 A.3h. 2) Detector voltage—Set detector operating voltage according
Before beginning calibration, ensure that the counting vacuum to manufacturer’s recommendations.
chamber is well sealed and has an adequate, consistent vacuum 3) Background—Background counts are the result of a contam-
source. Inadequate vacuum will result in a distorted alpha spec- inated sample chamber and cosmic, natural, and worldwide fall-
trum. An inconsistent vacuum can cause significant drift of the out in the detector shielding. Determine the detector background
alpha spectra. count using an appropriate volume of reagent-grade water in the
5) Continuing calibration (source check)—Verify detector effi- desired geometry. The background counting duration should be at
ciency and energy calibration stability. A mixed alpha-emitting least as long as the longest sample counting duration.
isotopic source containing at least two distinct peaks (see Sec- 4) Initial calibration—Establish a detector’s energy calibration,
tion 7020 A.3h allows the energy calibration to be confirmed by shape, and counting efficiency per sample geometry. Use a stan-
permitting identification of specific alpha-emitting radionuclides. dard source, as described in Section 7020 A.3h.
For criteria, see 7030 B.1f 6. 5) Continuing calibration (source check)—Verify the detector’s
6) Sample counting—Place prepared sample in the counting efficiency and energy calibration stability (Section 7020 A.3a).
chamber according to manufacturer’s instructions. Take the fol- Use a standard source, as described in Section 7020 A.3h.
lowing precautions: 6) Sample counting—Place the prepared sample in the count-
• ensure that the air in the counting chamber is slowly evacu- ing chamber and proceed according to the instrument manufac-
ated to the level of vacuum defined in the laboratory’s SOPs; turer’s instructions.
• count for a preset duration or preset count, to give the desired d. Gamma scintillation: A common gamma spectroscopy sys-
counting precision; tem is the sodium iodide, thallium-activated [NaI(Tl)] crystal sys-
• ensure that the sample is properly positioned on the sample tem using scintillation phenomenon. The high atomic number of
holder; and iodine in NaI gives good counting efficiency. A small amount of
• after counting, release vacuum slowly to minimize the risk of Tl is added to activate the crystal. The best achievable resolution
contaminating chamber and detector. is about 7% with the 137Cs gamma ray at 662 KeV gamma ray [in

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7030 COUNTING INSTRUMENTS - B. Description and Operation of Instruments

Table 7030:1. Energy Resolution for Various Detector Types with standards (e.g., 60Co, 137Cs, 207Bi, and 154Eu). Computer capabil-
Resolution at Given Energy ity is essential in both data reduction and complex sample analysis.
Detector 5.9 keV 122 keV 1332 keV
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Published Online: August 27, 2018


Revised: March 27, 2020
https://doi.org/10.2105/SMWW.2882.138 6

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