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Scintillation Crystals for PET*

Charles L. Melcher

CT! Inc., Knoxville, Tennessee

crystal,a fractionof the energylocalizeson the activator

In PET, inorganic scintillator crystals are used to record -y-rays
produced by the annihilation of positrons emitted by injected
tracers. The ultimate performanceof the camera is strongly tied
to boththe physicaland scintillationpropertiesofthe crystals.For
this reason, researchers have investigated virtually all known
scintillatorcrystals for possibleuse in PET.Despitethis massive
researcheffort, only a few differentscintillatorshave been found
that have a suitable combination of characteristics,and only 2
(thallium-doped sodium iodide and bismuth germanate) have
found widespread use. A recently developed scintillator crystal,
cenum-doped lutetium oxyorthosilicate,appears to surpass all
previously used materials in most respects and promises to be
the basisfor the next generationof PETcameras.
KeyWords: PET;scintillation crystals;lutetiumoxyorthosilicate
J NucI Med 2000;41:10511055
scintillator is a material with the ability to absorb
ionizing radiation, such as x- or rny-rays,and to convert a
fraction of the absorbed energy into visible or ultraviolet
photons. The conversion process typically takes place on a
time scale of nanoseconds to microseconds, thus producing
a brief pulse of photons corresponding to each rnl'-or x-ray
that interacts with the scintillator material. The light pulse,
the intensity of which is usually proportionalto the energy
deposited in the scintillator, is sensedby a photodetector and
converted into an electrical signal.
Scintillators may be liquid or solid, organic or inorganic,
and crystalline or noncrystalline. Organic liquid and plastic
scintillatorsoften are usedfor detectionof @3 particles and
fast neutrons. For the detection of x- and -y-rays, such as the
511 keV -1'-raysused in PET, inorganic single-crystal scintil
lators are used, becauseof their generally higher density and
atomic number, which lead to better detection efficiency.
A typical scintillator is a transparent single crystal in
which valence and conduction bands are separated by a band
gap of 5 eV or more. In a perfect crystal, free of defects or
impurities, there would be no electronic energy levels in this
gap. However, most scintillators are doped with an activator
ion that provides energy levels in the otherwise forbidden
band gap. After absorption of y-ray energy by the bulk
ReceivedJan. 7, 2000; revisionaccepted Feb. 9, 2000.
Forcorrespondenceor reprintscontact:CharlesL Melcher,PhD, CTI, Inc.,
810 InnovationDr.,Knoxville,TN37932.
*NOTE: FOR CE CREDIT, YOU CAN ACCESS THIS ARTICLE ON THE
SNMWEBSITE(http://www.snm.org)
UNTILDECEMBER
2000.
ions. Relaxation of the activatorionsresultsin the emission
of scintillation photons, typically around 4 eV, correspond
ing to visible blue light.
In the early years of PET, detectors were made of single
crystals ofthallium-doped sodium iodide (NaI[Tl]), individu
ally coupledto photomultiplier tubes(PMTs).With thediscovery
of bismuth germanate(Bi@Ge@O12 or BGO), most detector
designers converted to this material because of its much greater
efficiency for detecting y-rays.
Ablock detectorbecame the most
widely useddesign,in which a BGO block is segmentedinto as
many as 64 elements and coupled to 4 PMTs (1). Other
scintillators have included barium fluoride (BaF2 [2]), yttrium
aluminate (YA1O3[Ce]or YAP) (3), and cerium-dopedgadolin
mm oxyorthosilicate(Gd2SiO5[Ce]or GSO) (4). In recentyears,
a promising new material, cerium-doped lutetium oxyorthosili
cate (Lu25i05[Ce] or LSO) (5), has emerged and is likely
to be used widely in future generation PET scanners.
THE SCINTiLLATION PROCESS
The process whereby a scintillator converts the energy
deposited in it by a y-ray
into a pulse of visible (or ultraviolet
[UV}) photons includes 3 main steps. According to Lem
picki et al. (6), the overall efficiency (ri)
of the conversion
process may be characterized as the product of 3 factors:
vi
= I3SQ,
where 1@ is the conversion efficiency of the y-ray energy to
electron hole pairs, S is the transfer efficiency of the energy
held by the electron-hole pairs to the activator ions or other
luminescence centers, and Q is the quantum efficiency of the
luminescence centers themselves.
Robbins (7) demonstrated that @3 can be calculated from
thefundamental
physicalpropertiesof thescintillatorcrys
tal, including the electronic band gap, the high-frequency
and static dielectric constants,and the optic longitudinal
photonenergy.For many scintillatormaterials,theseparam
eters are well known; consequently, the conversion effi
ciency can be calculated with reasonable confidence. For
some newer scintillators,however, some of the parameters
are not known precisely, thus resulting in a significant
uncertainty in the calculated conversion efficiency.
Despite the obvious importance of 5, no model exists to
calculateit reliably. In fact, perhapsthe primary challengeof
current scintillator research is to develop an accurate model
of this crucial process.

SCINTILLATION CRYSTALS FOR PET Melcher 1051

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Qismeasured
bydirectly
exciting
thecenters
withUV TABLE 2
light, the energy of which matches the excitation energy of Physical Properties of Some Common Scintillator Crystals
the center. In this way, the electron-hole creation step and the
EffectiveCrystalDensity
energy transfer step are bypassed, and the efficiency of the
luminescence center itself can be observed directly. numberHygro
scopicRuggedCdWO47.9064NoNo
(glcm3)atomic
(cleaves
CHARACTERISTiCS OF ThE IDEAL SCINTILLATOR
easily)Lu2SiO5(Ce)(LSO)7.4065NoYesBi4Ge3O12(BGO)7.1375NoYesGd2S
The ideal scintillator would have a combination of several
physical and scintillation properties (Table 1). A high
detection efficiency for the -y-rays of interest requires both
high atomic number for a large photoelectron cross section (cleaves(GSO)easily)BaF24.8853NoYesCsF4.6453VeryNoCsl(Na)4.5154Ye
and high density for a large Compton-scattering cross
section. These are the 2 main interactions through which 511
keV rny-raysinteract with the scintillator crystals. For good
coincidence timing and high count-rate capability, a short
decay constant is required. In other words, the pulse of
scintillation photons must be as brief as possible. A high 817NoNo
light output allows a large number of crystal elements to be
coupled to a single photodetector, and good energy resolu
5,00010,000cc of scintillator crystals, the growth of large
tion allows a clear identification of full energy events. The
volumes of crystals at a reasonable cost must be feasible.
transmission ofthe scintillation light pulses into the photode
tector is best when the refractive index of the scintiulator
PROPERTIES OF COMMERCIAL SCINTILLATORS
material is similar to that of the entrance window and
coupling material, usually near 1.5. In some materials, color Because the ideal scintillator does not actually exist, one
centers may be easily produced by ionizing radiation, thus must look at the characteristics of materials that do exist and
impeding the transmission of the scintillation light through choose the one best suited to the application. Table 2 shows
the scintillator itself. Therefore, a resistance to this effect, the physical properties of some commonly available scintil
known as radiation hardness, is desirable. Some scintillators lator materials, listed in order of decreasing density. Both
are hygroscopic, i.e., they readily absorb water from the BGO and LSO have excellent physical properties. They
atmosphere and therefore require special packaging to have high density and atomic number that result in efficient
hermetically seal them. Nonhygroscopic materials have an detection of y-rays
and are also rugged and nonhygroscopic,
advantage, in that simpler packaging may be used. Mechani which allows relatively simple detector fabrication. Cad
cal ruggedness is desirable, because it makes fabrication of mium tungstate and GSO are also good candidates, except
small crystals easier. Because a PET scanner may use that both cleave easily, which makes detector fabrication
more difficult.
TABLE 1 Table 3 shows the scintillation and optical properties of
Properties of the Ideal Scintillation Crystal for PET some common scintillators, listed in order of increasing
decay constant. BaF2 has the shortest decay constant by far:
Crystalproperty Purpose 0.8 ns. Unfortunately, the emission is weak and located in
Highdensity High-y-raydetectionefficiency the far UV at 220 nm, which requires PMTs with more
Highatomicnumber High -y-ray detection efficiency expensive quartz windows. It also has a long secondary
Shortdecaytime Goodcoincidencetiming component of 600 ns. Cesium fluoride (CsF) has a very short
Highlightoutput Allowslargenumberof crystal
decay constant of 4 ns, but its intensity is so weak that this
elementsperphotodetector
Goodenergyresolution Clearidentificationof full scintillator is seldom used. LSO has the best combination of
energyevents a short decay constant, 40 ns, and high emission intensity. In
Emissionwavelengthnear Goodmatchto photomultiplier addition, it has no secondary decay component.
400 nm tuberesponse
Transparentat emission Allowslightto travelunim SCINTILLATORSUSEDIN PET
wavelength pededto photomultiplier
tube NaI(Tl) was discovered in 1948 by Hofstadter (8). It
Indexof refractionnear1.5 Goodtransmissionof light quickly became the scintillator of choice for radiation
fromcrystalto photomulti detection because of its high light output, i.e., efficient
pliertube
Radiationhard Stablecrystalperformance conversion of deposited -y-ray energy to scintillation pho
Nonhygroscopic Simplifiespackaging tons. The large light pulses are easily processed by conven
Rugged Allowsfabricationof smaller tional pulse-shaping electronics. The main disadvantage of
crystalelements NaI(Tl) is its low detection efficiency for y-rays
above 200
Economicgrowthprocess Reasonablecost keV, as a result of low density and moderately low atomic

1052 Ti@JouRNAL
OFNUCLEAR
MEDICINE

Vol. 41
No. 6
June2000
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TABLE 3
Scintillation and Optical Properties of Some Common Scintillator Crystals

decay decay emission of

refractionBaF20.860012220and3101.49CsF453901.48Lu2SiO5(Ce)
CrystalPnmary constant(ns)Secondary
constant(ns)Relative intensityEmission wavelength(nm)Index

(LSO)40754201.82Gd2SiO5(Ce)
(GSO)60600304301.85Nal(Tl)23010,0001004101.85Bi4Ge3O12

(BGO)300154802.15Csl(Na)630754201.84CaF2(Eu)900404351.44Csl(Tl)1

000455651.80CdWO4500020,000204802.20

number. At the energies typically used in SPECT (140 keV), crystalscleaveeasily.Thus, specialtechniquesare neededto
the detection efficiency of NaI(Tl) is satisfactory, and it is avoid cracking the crystal elements during cutting.
used almost exclusively in that application. However, for LSO offers the best combination of properties for PET of
higher energy applications, such as PET (511 keY), NaI('fl) any scintillator known today (13). It has high density and
has been replaced, for the most part, by materials with higher high atomic number for good -y-ray detection efficiency, a
density and atomic number. An additional disadvantage of short decay constant for good coincidence timing, and high
NaI(Tl) is that it is highly hygroscopic. As a result, a great light output that allows the use of many small elements per
deal of effort has gone into the development of hermetic PMT. In addition, it is mechanically rugged and nonhygro
packaging to protect the material from moisture in the scopic,thusallowing relatively simple fabricationof detec
atmosphere. tors. LSO has a low level of natural radioactivity as a result
BGO emerged in the early 1970s, with initial studies of the presence of 76Lu, but the counting rate from this
reported by Weber and Monchamp (9). Although the light isotope is a small fraction of the typical counting rates from
output of BOO is only about 15% of that of NaI(Tl), its the injected tracers; thus, it is not a significant problem for
dramatically higher detection efficiency, as a result of PET. LSO hasbeenusedin a high-resolution
braintomo
density almost twice that of Nal as well as a much higher graph (14), high-resolution animal tomographs (15), com
atomic number, has made it a very popular choice for the binedPETIMRIdetectors(16), andcombinedPET/SPECT
detection of radiation above a few hundred keV. PET is the cameras (17). Large-scale commercial production of LSO
major ongoing application of BGO crystals today, despite has been realized during 1999 (18), and widespread use of
the fact that their relatively long decay constant of 300 ns this scintillator is expected in the future.
limits coincidence timing resolution.
Scintillators with extremely short decay constants offer PROPERTIESOF SCINTILLATORSFOR PET
the possibility of time-of-flight PET, in which opposing Despite the investigation of virtually every known scintil
detectors measure the difference in the arrival times of a pairlator for possible use in PET, only 2 have seen widespread
of y rays. In this way, the location of the positron event can use so far, NaI(Tl) and BOO. A third, LSO(Ce), is expected
be localized along the line connecting the 2 detectors. Two to see widespread use in the future. In this section, the
possibilities that appear in Table 3 are CsF and BaF2. CsF properties of these 3 important scintillators are compared in
has very low light output and is very hygroscopic and, more detail.
consequently, has seenlittle use despiteits shortdecay One of the most important properties of a scintillator for
constant of 4 ns. BaF2has an even faster decay of less than 1 PET is y-raydetectionefficiency.Becauseof thedesireto
ns, greater light output, and is nonhygroscopic. Therefore, in shorten scan times and maintain low tracer activity, the
the early 1980s it was used in several PET scanners (10). crystals must detect as many of the -y-rays emitted as
However, because of its relatively low density and atomic possible. This is the primary reason for the popularity of
number, it eventually gave way to BGO. BGO. y-rays with energy of 511 keV interact with solid
One way to increase the spatial resolution of a tomograph matter primarily through 2 phenomena, the photoelectric
istocouplemultiplescintillatorcrystalswithdifferentdecay effect and the Compton effect. In the photoelectric effect, the
constants to a single photodetector. Pulse-shape discrimina -y-ray is absorbed by an atom that ejects an electron
tion is used to identify the crystal element of interaction. (photoelectron) and also produces either characteristic
GSO has been used in conjunction with BOO in this way for x-rays or Auger electrons. The end result is that the full
a high-resolution tomograph (4,11). A tomographic design energy of the y-ray
is absorbed. In Compton scattering, the
usingGSOexclusivelyhasalsobeenreported(12). Fabrica -y-ray loses a fraction of its energy to an electron through
tion of GSO detectors requires great care, because the scattering. The energy of the electron is likely to be absorbed

SCINTILLATION CRYSTALS FOR PET Melcher 1053

 Downloaded from jnm.snmjournals.org by on October 8, 2016. For personal use only.

in the crystal, whereas the scattered -y-ray may or may not be

absorbed. The distribution of energy between the electron
and the y-rayis determined by the scattering angle.
The detection efficiency of a detector may be character
ized by the fraction of incident -y-rays that are partially or
fully absorbed by it. For a detector of thickness x, exposed to
a mono-energetic beam of rny-rays,the initial y-ray intensity,
I@,is attenuated according to:
1(E) = I0(E) exp (six),
where I is the intensity of -y-rays passing through the
detector without interacting at all, and pi is the linear
attenuation coefficient. The y-rays that do interact in the
detector by depositing either their full or partial energy are
givenby:
A= 1 exp(px).
FIGURE2. Scintillationemissionspectraof Nal(TI),BOO,and
Thus, it is clear that the fraction of incident rny-raysthat are LSO(Ce),under-y-rayexcitation.
partially or fully absorbed is determined by the linear
attenuation coefficient (for an idealized geometry). Figure 1 near that wavelength, whereas BOO has a much weaker and
compares the linear attenuation coefficients for Nal, BOO, longer wavelength emission (480 nm) (Fig. 2). The intensity
and LSO. From these data, the advantagesof BOO and LSO of the scintillation emission strongly affects the number of
over Nal are clear. At 511 keV, p = 0.96 cm for BOO and crystal elements that can be coupled to a single PMT or,
1.1 = 0.87 for LSO, whereas for Nal, p is only 0.35 cm* stated another way, the ratio of scintillation elements to
Consequently, to achieve similar efficiency, Na! detectors electronic channels. With BOO, block detectors today use up
must be more than twice as thick compared with BOO and to 16 crystal elements per PMT, whereas LSO detectors use
LSO detectors. up to 144 crystal elements per PMT. Thus, LSO makes
In most PET scanners, the emission of the scintillation possible significant cost savings as a result of the reduced
crystals is converted to electrical signals by PMTs. To number of photomultipliers.
produce the largest signal, the scintillation emission should In PET, the decay constant of the scintillation emission is
be as intense as possible, and the wavelength of the emission very important, because singles count rates are typically
should match the wavelength of maximum photomultiplier very high, and coincidence resolving time should be as small
sensitivity. Because bi-alkali photomultipliers with glass as possible to reject unwanted random events. A short
entrance windows, the most commonly used type, have a scintillation decay constant is a benefit in both instances.
maximum sensitivity near 400 nm, it is advantageous for the Figure 3 compares the scintillation decay of NaI(Tl), BOO,
scintillator to have its emission maximum near this wave and LSO. BOO has the longest decay, 300 ns. The primary
length. Both Nal and LSO have intense emissions that peak decay constant of NaI(Tl) is somewhat shorter, 230 ns, but

1000

10@

I
100

10 p31
I.! 102

0.1 id @oo 2000 3000

10 100 1000 0

Energy(k&/) Time(nil

FIGURE 1. Total linear attenuation coefficients of Nal, BGO, FIGURE3. Decayofthe scintillation emissionof NaI(TI),BOO,
and LSO. and LSO(Ce),after excitationby -y-rays.

1054 Ti@ Jou@.r@i OF NUCLEARMEDICINE Vol. 41 No. 6 June 2000

 Downloaded from jnm.snmjournals.org by on October 8, 2016. For personal use only.
an additional secondary decay of several microseconds is
also present. The decay constant of LSO is several times
shorter, 40 ns, and no secondary component is present.
Because the quality of a PET image is strongly dependent
on the coincidence resolving time of the detectors, a figure
of merit that has been used for PET scintillators is the
number of photons emitted per nanosecond. In this way,
both the overall intensity of the emission as well as the
duration of the pulse are accounted for in 1 parameter.
Figure 4 compares the photons emitted per nanosecond for
Nal, BOO, and LSO. LSO has a large advantage over BOO
in this respect, because LSO's emission is both intense and
fast, whereas BOO's emission is much weaker and slower.
LSO is also better than Nal in this respect, becausealthough
Nal's emission is stronger than LSO, the decay constant is
more than 5 times longer.
FUTURE RESEARCH DIRECTIONS
Researchers continue to actively investigate potential new
scintillator materials, because a tomograph's performance
depends so strongly on the characteristics of the detectors.
Most of the effort has focused on high-density and high
atomic-number materials as well as materials with poten
tially very short decay constants. Surveys of large numbers
of candidates (19) have failed to identify any practical
scintillators for PET. Recent research, therefore, has shifted
toward computational efforts to model potential materials
(20,21). Hopefully, an improved understanding of the under
lying physics of scintillation processeswill lead to the
ability to predict the characteristics of new scintillator
materials without actually synthesizing them.
In addition to searching for new scintillator materials,
investigators have combined known scintillators in novel
ways, such as phoswich detectors, which combine 2 dissimi
lar scintillators in the same detector. For instance, layers of
LSO and NaI(Tl) have been combined to make a camera that
1@@uec)
FIGURE 4. Comparisonof rate of scintillation emission(pho
tons emitted per nanosecondafter excitation)for NaI(Tl), BOO,
and LSO(Ce).
provides both PET and SPECT capability (18). The LSO
layer is used for PET imaging and the NaI(Tl) layer is used
for SPECT imaging. Similarly, researchershave constructed
prototype detectors of LSO and YSO for the same purpose
(22).
ACKNOWLEDGMENTS
The author is grateful to Lars Eriksson and Mike Casey
for several useful discussions.
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Scintillation Crystals for PET

Charles L. Melcher

J Nucl Med. 2000;41:1051-1055.

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