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☆
becomes prominent when the energy of the photon is less than about 200 keV,
ENERGY (keV)
because, at energies above 200keV, the iodine escape peak would fall within the width of the photopeak, due to the small differences between the two peaks.

8.4.6 Positron Annihilation Peak

γ-rays with energy greater than 1.02MeV may undergo pair production in the detec­tor in which a positive–negative electron pair is produced. The β+-particles are anni­hilated to produce two 511-keV photons, which appear as photopeaks in the γ-ray spectrum. If, however, one of the 511-keV photons escapes from the detector, then a peak, called the single-escape peak, corresponding to the primary photon energy minus 511keV, will appear in the spectrum. If both annihilation photons escape, then a double-escape peak results, corresponding to the primary photon energy minus 1.02 MeV. Larger detectors can prevent the escape of the annihilation radiations.

8.4.7 Coincidence Peak

A coincidence or sum peak results when more than one photon is absorbed simulta­neously in the detector to be considered as a single event. The peak equals the sum of the energies of the photons. Such situations occur with radionuclides that have short-lived isomeric states and thus emit γ-rays in cascade. For example, 171- and 245-keV photons, which can result in a sum peak of 416keV (Fig.8.5). Sum peaks are also caused by counting high-activity samples in which two photons may strike the detector at the same time. These peaks can be reduced by counting the samples at larger distances between the source and the detector or by using smaller detectors so that the likelihood of two photons striking the detector at the same time is reduced. In the case of high-activity samples, the level of activity has to be reduced either by dilution or allowing to decay, in order to reduce the sum peak.
111
In emits
Fig. 8.5 A spectrum of
111
In with 171- and 245-keV photons showing a coincidence (sum) peak at 416keV
70
60
50
40
30
20
10
80 160 240 320 400

8.5 Liquid Scintillation Counter

Scaler
Freezer
Low-energy β−-particles are normally absorbed within the source and in the window and walls of the detectors, and therefore β−-emitters are difcult to detect in gas or solid detectors. For this reason, β−-emitting radionuclides are counted using the liquid scintillation technique in which the radioactive sample is mixed with a scin­tillating material. A sample vial containing the liquid scintillator and the radioactive sample of interest is placed between two PM tubes connected in coincidence (Fig.8.6). Each PM tube receives the light photons emitted by the interaction of the
β−-particle with the scintillator and converts them into a pulse, which is further
amplied by an amplier. The amplitude of the pulses is proportional to the energy of the β−-particles. The amplied pulses are then delivered to the coincidence circuit that contains a PHA to analyze the pulse height for acceptance. A count is registered in the scaler if two pulses of the same height are recorded in both PM tubes simul­taneously. Such coincidence counting reduces the background counts due to noise, including terrestrial and cosmic radiations, radioactive patients, etc.
The liquid scintillation solution is prepared by dissolving a primary scintillating solute or uor and often a secondary uor in a solvent. The radioactive sample is added to and thoroughly mixed with the scintillating solution for counting. The primary uors include 2,5-diphenyloxazole (PPO), 2,5 bis-2-(5-T- butylbenzoxazolyl)-thiophene (BBOT), and p-terphenyl, of which PPO is most commonly used in a concentration of 5g/L.
Toluene, xylene, and dioxane are the most common solvents that easily dissolve the primary uor and often the radioactive sample, which is a requirement for a good solvent. These solvents, however, are poorly miscible in water, and therefore their disposal in the sewer system is restricted. For this reason, biodegradable
Amplifier
Pre-
amplifier
Fig. 8.6 A schematic diagram of a liquid scintillation counting system. Light photons emitted from the sample strike the two photomultiplier tubes to produce pulses. Only coincident pulses are counted
Coincidence
Circuit
Radioactive sample
Amplifier
PM tubePM tube
Pre-
amplifier
solvents such as linear alkylbenzene and phenyl xylyl ethane are widely used. Counting vials are usually glass or plastic, but the latter is not used when toluene or xylene is used as a solvent because the solvent tends to dissolve plastic.
When radiations pass through the solvent, electrons are released from the solvent molecules after absorption of radiation energies. These electrons transfer energy to primary uor molecules, which then emit light photons for further processing by PM tubes and associated electronics. The wavelength of these light photons may be somewhat shorter than required for the spectral sensitivity of the photocathode of the PM tube. This mismatch is rectied by adding a secondary uor or solute, called the wavelength shifter, to the scintillating solution. The wavelength shifter absorbs the light photons emitted by the primary uor and reemits them with a longer wave­length, which is more suitable for the photocathode of the PM tube. The compound 1, 4-bis-2-(5-phenyloxazolyl)-benzene (POPOP) is most commonly used as a sec­ondary solute in a concentration of about 0.1%.
An attempt is always made to keep the radioactive sample in solution in the liq­uid scintillator. Solubilizing agents are added to improve dissolution of specic samples, and the common example is the hydroxide of Hyamine 10-X used in counting tissue samples.

8.5.1 Quenching

In liquid scintillation counting, quenching is a problem caused by interference with the production and transmission of light, which ultimately reduces the detection efciency of the system. Quenching can be of the following types:
1. Chemical type, resulting from interference in energy transfer by substances such
as samples or extraneous materials (e.g., dissolved O2).
2. Color type, resulting from absorption of light photons by colored substances,
such as hemoglobin, before striking the PM tube.
3. Dilution type, resulting from relatively large dilution of the scintillation mixture,
in which case many light photons may be absorbed by the diluted sample.
4. Optical type, resulting from absorption of light by a dirty vial containing frost or
ngerprints.
Quenching must be corrected to obtain accurate counting of samples, and three methods have been adopted for this purpose, namely, internal standard method, channel ratio method, and external standard method. The readers are asked to refer to physics books for details of these methods.
A problem with liquid scintillation counting is the noise due to spontaneous ther­mal emission of electrons from the photocathode of the PM tube. Background noise also arises from the interaction of light with scintillation solution. Thermal emission of electrons is reduced by refrigeration of the counting chamber to keep the PM tubes at low temperature. But the coincidence counting is the most effective method to reduce the noise.
The liquid scintillation counting systems are provided with automatic sample
E
nX
FWHM
E
100
changers for counting as many as 500 samples. Also, one to ve PHAs are available on a liquid scintillation counter, so that β−-particles of different energies can be counted simultaneously by using different baselines and windows on each PHA. The
β−-emitters, 3H, 14C, 32P, and 35S, are commonly detected by liquid scintillation
counting. Whereas, the counting efciencies of 3H (E (E
=1.71MeV) are ∼60–70% and ∼100% respectively, they are negligible for
max
 = 0.018 MeV) and 32P
max
γ- and x-rays.
8.6 Characteristics ofCounting System
Detection of radiation and therefore counting of radioactive samples is affected by different characteristics of the detector and the associated electronics. The follow­ing is a discussion of these properties.

8.6.1 Energy Resolution

As already mentioned, even though γ-rays of the same energy are absorbed in the NaI(Tl) detector by the photoelectric effect, pulses of different amplitudes are pro­duced because of the statistical variations in the production of light photons in the detector and photoelectrons and electrons in the PM tube. This results in the broad­ening of the photopeak. The width of the peak or the sharpness of the peak (i.e., the energy resolution of the detector) predicts the ability of the NaI(Tl) spectrometer to discriminate between the γ-ray photons of dissimilar energies. A similar situation exists for semiconductor detectors where the number of ionizations may vary from one γ-ray to another of the same energy, leading to the broadening of the peak.
The energy resolution of a system is given by the full width at half-maximum (FWHM) amplitude of the photopeak expressed as a percentage of the photon energy as follows:
nergyresolutio
%
(8.1)
where Eγ is the energy of the γ-ray photon. In Fig.8.7, FWHM is 55 keV for the 662-keV peak of
137
Cs; therefore,
Energy resolution%
55
662
.%
83
100
The energy resolution depends on the photon energy. The higher the photon energy, the better the energy resolution (i.e., smaller FWHM), because of the decrease in the percentage of statistical variations in the pulse production. The energy resolution of NaI(Tl) detectors is about 7–10% for the 662-keV γ-ray of
70
ENERGY (keV)
V
Fig. 8.7 The full width at
Efficiency ff fN
ipgi
half maximum (FWHM) of the 662-keV γ-ray of in a NaI(Tl) detector
137
Cs
60
50
40
30
20
10
137
Cs and 10–14% for the 140-keV γ-ray of
FWHM =
99m
Tc. In contrast, the energy resolution
800 700 600 500 300 200 100 400
∆E = 55 ke
in Ge(Li) detectors is about 0.42% for 140-keV γ-rays and about 0.2% for photons of more than 1MeV.

8.6.2 Detection Efficiency

The detection efciency of a counter is given by the observed count rate divided by the disintegration rate of a radioactive sample. The count rate of a sample differs from the disintegration rate because of several factors. Radiations from a source are emitted isotropically around 4π steridians, but only a fraction of all photons emitted strikes the detector, depending on the solid angle subtended by the detector on the source. Also, only a fraction of all photons striking the detector may interact in the detector and produce pulses. Only a fraction of all pulses produces a single photo­peak. Furthermore, the count rate is affected by the abundance of a particular radia­tion from a radionuclide. Considering these factors, the overall counting efciency of a counter for a radiation is given by the following expression:
(8.2)
where fi is the intrinsic efciency; fp is the photopeak efciency, or photofraction; fg is the geometric efciency; and Ni is the abundance of the radiation in question. Ni is available in literature on Tables of Isotopes.
8.6.2.1 Intrinsic Efficiency
The fraction of all radiations of a given type and energy impinging on the detector that interacts with it to produce pulses is called the intrinsic efciency, fi, of the detector:
No of radiations detected bythe detector
Allcounts under the photopeak
Gamma ray energy (keV)
fi=
.
No of radiations
.
impingingon the detector
Allcounts under the entire spect=rrum
No of radiations impinging on the detector.
(8.3)
It includes all photons undergoing both photoelectric absorption and Compton scattering. Intrinsic efciency depends on the type and energy of the radiation and the linear attenuation coefcient (μ) and thickness of the detector. The dependence of intrinsic efciency on the photon energy and the detector thickness is illustrated in Fig.8.8. The value of fi is almost 1 for low-energy γ-rays and thicker detectors. The fi tends to 0 for high-energy γ-rays and thinner detectors. These conditions apply to all solid scintillation detectors. The intrinsic efciency of gas detectors is almost unity for α- and β-particles but is about 0.01 (1%) for γ- and x-rays.
8.6.2.2 Photopeak Efficiency or Photofraction
The fraction of all detected γ-rays that contributes only to the photopeak is called the photopeak efciency, or photofraction (fp). It is given as the total photopeak area divided by the total area under the entire spectrum:
fp=
All photons detected by the deetector
(8.4)
This value is affected by all factors that inuence photoelectric effect, such as the size and composition of the detector and γ-ray energy, but is primarily determined by the discriminator settings on the PHA. The fp increases with increasing window width of the PHA.
Fig. 8.8 Dependence of intrinsic efciency on photon energy and detector thickness
100
75
50
25
Nal(TI) thickness
1.3 cm
0.6 cm
70 140 210
280
8.6.2.3 Geometric Efficiency
r
R
2
4
a
b
c
Radiations from a source are emitted uniformly with equal intensity in all direc­tions. If a source of radiation is placed at a distance from a detector, then only a fraction of all radiations emitted from the source will be detected by the detector. This fraction is determined by the solid angle subtended by the detector on the source. The geometric efciency, fg, is equal to the number of radiations striking the detector divided by the total number of radiations emitted by the source.
Thus,
No of radiations striking the detector
fg=
Total number of r
.
aadiations emittedbythe source
(8.5)
For a circular detector with radius r, it is equal to the area πr2 of the detector divided by the total spherical area 4πR2, where R is the distance between a point source S and the detector D (Fig.8.9).
f
g
2
(8.6)
As the distance R between the source and the detector increases, the fg decreases, according to the inverse square law, that is, fg∝1/R2 (Fig.8.9a). Thus the fg at 2R is one fourth of the fg at R. The value of fg increases with the size of the detector. Also, the nite size of the radiation source affects the fg values. When the source and the detector are in close contact, the fg tends to be about 50% (Fig.8.9b). In the case of gamma well counters and liquid scintillation counters, the
fg approaches 100% (Fig.8.9c).
Fig. 8.9 Illustration of geometric efciency, fg, of a detector D with a circular
2
area, πr
, where r is the
radius of the detector. (a) The detector D placed at a distance R from the point source S has an f times greater than the f when the detector is placed at a distance 2R. (b) When the source and the detector are in close contact, the f is about 50%. (c) When the source is well inside the detector as in a well counter, the f approaches 100%
four
g
g
g
g
S D
S
SD
R
r
2R
r
D D

8.6.3 Dead Time

RR R
to o
/1
Each counting system takes a certain amount of time to process a radiation event, starting from interaction of radiation with the detector all the way up to forming a pulse and ultimately recording it. The counter remains insensitive to a second event for this period of time, that is, if a second radiation arrives during this time, the counter cannot process it. This period is called the dead time. When the counter recovers after this period, only then can a second radiation be detected. Thus the second event arriving during the dead time is lost. Counts lost during the dead time are called the dead-time loss. In scintillation detectors, radiations may arrive at the same time and be processed simultaneously to form a single event of amplitude that is equal to the sum of the amplitudes of both events. This is referred to as pulse pileup. If one or both of the events were photopeaks originally, then the combined peak will fall outside the PHA window setting and be lost. Dead time loss at high count rates is a serious problem for any counting system and is more so for scintil­lation cameras due to pulse pileup (see Chap. 11).
The dead time of a counting system may arise from different components of the entire counting system: detector, PHA, PM tube, scaler, computer interface, and so on. While Geiger–Müller (GM) detectors have a longer dead time of 80–500μs, the typical values for NaI(Tl) and semiconductors are of the order of 0.5–10μs and for liquid scintillators, ∼0.1–1 μs (Cherry etal. 2012).
Based on how successive pulses are processed owing to the dead time, the count­ing systems fall into two categories: paralyzable and nonparalyzable. In paralyz- able systems, each event sets its own dead time, even if it arrives within the dead time of the previous event and is not counted. Each event prolongs the dead time induced by the previous event, and thus adds to the total dead time of the system, whereby a paralyzable system can become totally unresponsive to process events if the count rate of the source is very high. On the other hand, in nonparalyzable sys­tems, the instrument remains insensitive to successive events for a period of time equal to the dead time, and these events are lost. But unlike paralyzable systems, the dead time is not changed or lengthened. When the system recovers after the detec­tion of the rst event, only then is the second event processed and detected. The two types of dead time losses are illustrated in Fig.8.10.
The paralyzable and nonparalyzable systems can be represented by mathemati­cal relationships among the observed count rate R τ. For nonparalyzable systems,
, true count rate Rt, and dead time
o
(8.7)
and for paralyzable systems,
R
-
t
RRe
0
t
(8.8)
Different components of a radiation detection system can have either paralyzable or nonparalyzable dead time. Scalers and pulse-height analyzers are nonparalyzable systems, whereas radiation detectors themselves are paralyzable systems.
TRUE COUNT RATE
NONPARALYZABLE
Fig. 8.10 Plot of observed count rates versus true count rates indicating the dead time loss in paralyzable and nonparalyzable systems
2.0
1.5
1.0
0.5
6
10
×
0.51.5 2.0
1
PARALYZABLE
Scintillation cameras have both paralyzable and nonparalyzable components of dead time. As can be seen from Eq. (8.8), the radiation detectors become totally paralyzed at very high count rates giving no reading.
Dead time loss is a serious problem for a counting system at high count rates. Therefore, either count rates must be lowered or corrections must be made to the observed count rates. There are several methods to determine or correct for dead time. An empirical method is to plot the observed count rates as a function of increasing concentrations of known activity. From the plot and Eqs. (8.7) and (8.8), the dead time is calculated for the nonparalyzable or paralyzable system. For sub­sequent measurements of unknown samples, correction is made to compensate for the dead time loss giving true count rates. Another method uses two radioactive sources, which are counted in the counter individually and together. From these three measurements, one can calculate dead time using appropriate equations (see Cherry etal. 2012). Various techniques, such as use of buffers, in which overlapping events are held off during the dead time, use of pulse pileup rejection circuits, and use of high-speed electronics have been employed to improve the dead time correction.

8.7 Gamma Well Counter

The gamma well counter consists of a NaI(Tl) detector with a hole in the center for a sample to be placed and associated electronics such as a PM tube, preamplier, amplier, PHA, and scaler–timer. Placing a radioactive sample in the central hole of the detector increases the geometric efciency (almost 99%) and hence the counting efciency of the counter. The NaI(Tl) detectors have dimensions in the range of 5-cm diameter × 5-cm thick to 23-cm diameter × 23-cm thick. Smaller detectors are used for low-energy γ-rays (less than 200keV), and larger detectors are used for high-energy γ-rays. Most well counters are shielded with about 8.5-cm thick
Radioactive
Fig. 8.11 A schematic diagram of a NaI(Tl) well counter with a PM, photomultiplier tube
sample Nal (TI) Crystal
circular lead ring to reduce background from cosmic rays, natural radioactivity such as 40K, or background activity in the work area. A typical well counter detector is shown in Fig.8.11.
8.7.1 Calibration ofWell Counter
It is essential that the dial settings of the discriminators on the PHA are calibrated so that the dial readings correspond directly to the pulse height (i.e., the energy of the γ-ray photon); that is, the dial readings can be read in units of keV.This calibra­tion is called the high-voltage or energy calibration of the well counter. The energy calibration is carried out by using the 662-keV photons of
137
Cs source in the well counter, the lower and upper discriminator levels are set at 640 divisions and 684 divisions, respectively, thus assigning the center of the pho­topeak at 662 divisions corresponding to the 662-keV γ-ray. Starting from low val­ues, the high voltage is increased in small increments for a given amplier gain until the observed count rate reaches a maximum. The high voltage at the maximum count rate is kept as the operating voltage for subsequent counting of photons of different energies. The discriminator dials are then said to be energy calibrated; for example, each dial unit corresponds to 1keV at an amplier gain of 1. Thus, the
99m
center of the 140-keV photopeak of
Tc can be set at 140 divisions of the discrimi­nator setting, with lower and upper values set as desired. After calibration, well counters should be checked regularly for any voltage drift using a long-lived source, such as
137
Cs.
137
Cs. After placing a
8.7.2 Counting inWell Counter
For relative comparison of count rates between samples, the well counter does not need to be calibrated, provided all samples for comparison have the same volume. In radioimmunoassays, ferrokinetics, blood volume, red cell mass measurements, a standard of the same geometry (volume) and with relatively the same activity is counted along with all samples, and then a comparison is made between each