Characterization and optimization of pyroelectric X-ray sources

using Monte Carlo spectral models

Michael Klopfer, Thomas Wolowiec, Vladimir Satchouk, Yahya Alivov, Sabee Molloi
n
Department of Radiological Sciences, Medical Sciences B, 140, University of California, Irvine, CA 92697, USA
a r t i c l e i n f o
Article history:
Received 5 April 2012
Accepted 23 May 2012
Available online 13 June 2012
Keywords:
Ferroelectric
X-ray source
Pyroelectric
X-ray anode
Brachytherapy
a b s t r a c t
Pyroelectric X-ray sources produce emission through bulk heating of a ferroelectric crystal. In this
study, a least-square based systematic curve tting of X-ray emission to predicted models is used to
generate an equivalent monoenergetic incident electron energy to simplify further X-ray source
optimization. The measured X-ray spectrum of a 1 cm
3
lithium tantalite crystal cycled over 140 K are
shown to be approximated by those of an 85 keV monoenergetic electron beam. Using monoenergetic
electron sources, common congurations for transmission and directional X-ray sources are simulated
using electron targets comprised of gold, silver, copper, molybdenum and tungsten. X-ray production
efciency depends on target material selection, incident electron energy, and target thickness for both
transmission and reection geometries. At 20 keV, silver produced 69.7% more ux was in comparison
to copper, the least efcient target material at this energy. Conversely, at 85 keV copper outperformed
silver, the least efcient target material at this energy, by 21.6%. Pyroelectric X-ray sources can be
improved for ux and energy tuning through the use of modeling and target design. Continued
development of pyroelectric X-ray sources can lead to wide scale implementation for industrial X-ray
uorescence and medical therapeutic applications.
& 2012 Elsevier B.V. All rights reserved.
1. Introduction
Pyroelectricity results from a spontaneous depolarization upon
bulk temperature change in a pre-polarized ferroelectric crystal,
resulting in potential differences up to several hundred keV [18].
Electron emission due to FowlerNordheim tunneling of low
pressure gas molecules near the crystal surface and correspond-
ing eld acceleration has been used to generate X-rays when
accelerated electrons interact with a target [913]. Prior studies
that have demonstrated radiographic imaging and X-ray uores-
cence analysis capabilities of pyroelectric sources indicate chal-
lenges for both ux and X-ray peak energy [1420]. During
emission, the generated crystal surface charge is depleted. Corre-
spondingly, the predicted maximum charge and electron poten-
tial do not directly translate into maximum observed photon
energy as predicted by the DuaneHunt law for maximum
bremsstrahlung photon energy [21]. Previous reports indicated a
swept, packeted monochromatic emission in X-ray energy
[22,23]. Due to the low current of pyroelectric sources, once
electrons are generated, an efcient electronphoton conversion
is necessary to maximize the total ux. The efciency of X-ray
production is dependent on incident electron energy, target
thickness, and atomic number (z). Increased target thickness
results in both increased X-ray conversion and self-attenuation
of produced photons; therefore optimization of both target
thickness and atomic number is required to maximize the X-ray
ux. Two common congurations are used for X-ray generation,
transmission and directional geometries (Fig. 1a and b). While
general studies of target design for X-ray tubes have been
performed, no systematic studies have been performed to opti-
mize the efciency of a practical pyroelectric X-ray source [24]. In
this work, we studied the effect of target thickness on X-ray
emission efciency by Monte Carlo simulations using the package
EGSnrc [25]. To achieve this goal, a pyroelectric crystal was
modeled as emitting a single monochromatic electron. This
hypothesis is validated using a systematic curve tting between
a Monte Carlo electronphoton conversion chain and an experi-
mental model. Once a reasonable expectation for incident elec-
tron energy is determined, Monte Carlo modeling is used to
simulate the X-ray emission properties for a range of common
X-ray target materials used in low power X-ray sources at various
congurations and thicknesses. In this report we rst introduce
simulation details and experimental setup used to measure
pyroelectric X-ray spectrum. This is followed by presentation of
spectral determination and predictive models for simulated target
congurations.
Contents lists available at SciVerse ScienceDirect
journal homepage: www.elsevier.com/locate/nima
Nuclear Instruments and Methods in
Physics Research A
0168-9002/$ - see front matter & 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.nima.2012.05.065
n
Corresponding author. Tel.: 1 310 502 1971; fax: 1 949 824 0455.
E-mail address: symolloi@uci.edu (S. Molloi).
Nuclear Instruments and Methods in Physics Research A 689 (2012) 4751
2. Materials and methods
2.1. Monte Carlo modeling of input electron energy
The electronphoton transport simulation package EGSnrc was
used for all Monte Carlo simulations [25]. Two types of X-ray
generation designs were simulated: a directional-geometry X-ray
source as shown in Fig. 1a, and a target perpendicular to the
electron beam as shown in Fig. 1b. A total of 10
8
photons at 30,
60, 80, 85, 90, 100, and 120 KeV were directed in a 0.5 cm
2
diameter collimated beam toward a 3 mm thick, 20 mm
2
copper
target placed at 201 with respect to the cathode. Beam ltration
was determined by experimental setup and was modeled by
15 cm of air, 0.25 mm of aluminum, and 2 mm of borosilicate
glass. A 5 cm
2
ideal detector is modeled by the scoring plane.
Collected photons were normalized by peak energy for compar-
ison. Mean spectral energy was determined by a histogram
average of counts with respect to energy. Peak ux energy is
determined by a maximum value search after a 2 keV wide low
pass kernel is used to remove characteristic X-ray uorescence
peaks from simulated data. Peak energy was determined by the
energy corresponding to threshold of a signal-to-noise ratio of
5 against the background [26].
2.2. Modeling of multiple anode congurations
Alternative anode congurations and materials were modeled
and evaluated for X-ray conversion, efciency, and spectral
characteristics:
Ef f icency
E
incident
P
detected
1
In addition to prior criterion metrics, conversion efciency (Eq.
1) is dened as the fraction of detected photons (P
detected
) at the
scoring plane to the total incident electrons (E
incident
). A cutoff of
1 keV was used to discard low energy photons. To preserve
universality of results, no ltration was modeled between the
emission source and the scoring plane. Common high-z X-ray
anode materials, including copper, molybdenum, gold, silver, and
tungsten, were chosen based on prior use in industrial or medical
X-ray sources. Directional (Fig. 1a) and transmission (Fig. 1b)
geometries were tested. Scoring planes were simulated as 20 cm
2
planes immediately adjacent to the X-ray target to allow a large
acceptance angle to approximate 2p detector geometry. Direc-
tional targets were all modeled to have 2 mm thickness. This
thickness was chosen to block all transmission electrons for all
evaluated energies and can be modeled as innitely thick.
Transmission geometry target thicknesses were varied between
1 and 10 mm. The substrate for modeled transmission geometry is
omitted to eliminate the ltration effect generated by additional
material in the photon beam line. Monoenergetic electrons with
energies of 5, 8, 10, 12, 15, 20, 25, 30, 60, 85, 100, and 120 keV
were simulated to model an energy range that is observed or
modeled in prior pyroelectric experiments [19,27].
2.3. Experimental pyroelectric X-ray emission source
An experimental reference spectra were generated from a
directional geometry pyroelectric X-ray emission source (Fig. 2)
constructed from a 1 cm
3
lithium tantalate monolithic crystal
with the Z-polarized face epoxy-bonded to a grounded 2 O 20 W
resistor such that a negative polarity with respect to the electron
target is achieved during heating. Working vacuum level was
regulated with an adjustable leak of air to maintain 820 mTorr
dynamic pressure in accordance with documented parameters to
maximize gas amplication of electron emission [28]. Generated
electrons from the surface of the pyroelectric crystal pass an
empirically determined 0.6 cm gap to allow self-focusing and
strike a 2 mm thick copper electron target mounted at 201 with
respect to the incident beam [2,22]. Generated X-rays were
passed through a 2.0 mm thick, 76 mm square borosilicate (Corn-
ing 7740) window inside a stainless steel vacuum chamber. An
Ortec NaI(Tl) detector and Ortec Trump-32 MCA were used for
spectra collection. A spacing of 50 cm was chosen between the
detector crystal face and the window of the chamber to reduce
detected multi-photon events. A Keithley 614 picoammeter was
used to measure anode current. Thermal cycling to a difference of
140 1C was provided by use of a battery-based thermostatic
controller which raised the temperature at 1.2 1C/s until the
desired temperature difference was achieved. Passive cooling to
ambient temperature was allowed between runs. X-rays emitted
during cooling were not studied in this experiment. Spectra and
current collection began at initiation of heating current and
ceased when X-ray emission stopped after nal temperature is
reached. To improve counting statistics, spectra were averaged
over 5 identical runs using identical experimental parameters.
Background and energy-dependent detector quantum efciency
corrections were made post-data averaging. Mean spectral
energy, peak energy, and peak ux energy were determined with
identical methods of those used in simulation.
Fig. 1 Fig. 2
M. Klopfer et al. / Nuclear Instruments and Methods in Physics Research A 689 (2012) 4751 48
3. Results
3.1. Experimental validation of spectra
In Fig. 3, both simulated and experimental X-ray spectra are
shown. As seen from this gure, the experimental X-ray spectrum
from a LiTiO
3
pyroelectric crystal under measured conditions
described above is shown. This spectrum had a peak energy at
27.6 keV and spanned until maximum energy at 93 keV. As can be
seen from this gure, all simulated spectra showed close spectral
correlation with experimental data, indicating that the initial
assumption of a monochromatic electron beam can be used to
approximate the swept monochromatic electron beam generated
by a pyroelectric crystal. Table 1 summarizes the characteristics
of all X-ray spectra extracted from Fig. 3.
A goodness-of-t analysis based on point-by-point least-
square RMS error (Table 1) was tested between candidate mono-
chromatic spectra at a given energy. The result showed 85 keV as
the closest representation of the measured spectra with a mini-
mum absolute error of 0.23 (Fig. 3). The generated spectra
underestimated the peak energy as observed at 93 keV by 8 keV
while overestimating the spectral peak energy and mean spectral
energy by 2.7 keV and 1.7 keV, respectively. As comparison is
made above the Compton edge for the experimental data, char-
acteristic X-rays emitted by copper are not compared such that
the spectral peak energy and ux peak energy are equivalent in
this comparison.
3.2. Optimization of electron target parameters
Simulation of directional X-ray design parameters demon-
strated that at low energies (below 30 keV), silver outperformed
other tested materials with respect to X-ray conversion efciency,
while at high energies copper performed the best. At 20 keV an
11.3% improvement was seen by silver over copper. At 85 keV, a
54.7% improvement is seen by copper over silver. All other tested
materials performed between copper and sliver across the entire
energy range. For transmission geometry, tested targets were
used with optimum thickness for each tested energy. At 20 keV,
69.7% more ux was produced in comparison to copper, the least
efcient target material at this energy. At 85 keV, copper out-
performed silver, the least efcient target material at this energy,
by 21.6%. In Figs. 4 and 5, the calculated efciency of X-ray
emission of sources for different target materials in both direc-
tional and transmission geometries are shown. As different
thicknesses of different transmission targets have a pronounced
effect on X-ray emission, only optimized values are shown in
Fig. 5. In Fig. 6, the effect of thickness on efciency as demon-
strated at 20 and 85 keV incident electrons is shown. In Fig. 7, the
optimized thickness values for the tested materials across multi-
ple energies are shown. In Fig. 8, the produced spectra for an
incident 100 kev monoenergetic electron beam and a common
anode thickness of 5 mm are shown.
4. Discussion
As used directly for medical imaging or brachytherapy appli-
cations, optimization of electronphoton conversion and spectral
energy properties is critical to device usefulness [29]. Likewise
XRF applications also benet from improved X-ray ux for
shortened detection times and increased material sensitivity.
Prediction of acceleration potential (V) due to the pyroelectric
effect can be done using a capacitive model [23]. In an accelerator
conguration, a paired capacitor set is used to represent the
distance of the gap (d
gap
) that exists between the crystal surface
and the opposing electrode:
V
Q
C
crystal
C
gap

g DT
e
o
e
cr
1=d
cr
e
o
1=d
gap
2
where Q is the generated charge, g is the pyroelectric constant of
the material, and DT is the temperature gradient which the crystal
is cycled across. C
crystal
and C
gap
are the capacitance of the system
components, e
o
is the permittivity of free space, e
cr
is the crystal
relative permittivity, and d
cr
is the crystal thickness. When
Fig. 3
Table 1
Maximum energy
(keV)
Mean spectral
energy
Flux peak
energy
Absolute RMS
error
Experimental 35.8 27.6
60.0 30.2 24.9 0.73
80.0 36.3 29.1 0.38
85.0 37.5 30.3 0.23
90.0 40.1 30.7 0.36
100.0 43.5 31.2 0.62
120.0 48.5 33.9 0.83
Fig. 4
M. Klopfer et al. / Nuclear Instruments and Methods in Physics Research A 689 (2012) 4751 49
approximating the surface charge alone, the value of C
gap
is
assumed to be negligible [8]. The observed differences in spectral
characteristics and underestimation of both current and voltage
were noted in prior estimation models [27]. From this model, the
crystal used in this study would produce 604 keV potential across
the crystal and 444 keV with respect to the electron target, placed
at a distance of 0.6 cm. This result is divergent from maximum
photon energy of 93 keV that was observed in the experimental
spectrum (Fig. 3). This constitutes observing only 20.9% of the
maximum predicted electron energy through the bremsstrahlung
and transport process. A total of 3.1210
12
accumulated elec-
trons were measured as averaged over 5 cycles constituting only
20.2% of the predicted 1.5410
13
generated electrons per cycle.
While conrmation of low numbers of high energy electron
emission has been made in other experiments [23], the inherent
inefciency of the bremsstrahlung process hinders observation of
corresponding high energy photons matching the incident elec-
tron energy as predicted by the DuaneHunt law [21,30].
In conventional high ux X-ray tubes, heat capacity of the
anode must be taken into account. This traditionally limits the
anode material choice to tungsten or molybdenum. For pyro-
electric sources, the low incident electron ux can allow alter-
native elements with comparably low melting points such as
copper, gold, and silver. An increased atomic number leads to
higher bremsstrahlung generation. X-ray conversion from the
bremsstrahlung process can be estimated over a wide energy
band through the following relationship:
E
bremsstrahlung
E
thermal

E
k
Z
820,000
3
where E
k
is the incident electron energy in keV and Z is the
effective atomic number of the target material [26]. Correspond-
ingly, a higher elemental Z number leads to increased atomic
mass and mass attenuation [31]. As photons are generated within
the bulk of the material, attenuation leads to reduction of emitted
photons. The effects of Compton and Rayleigh scatter also lead to
the complication of calculation for anode efciency as energy and
path length are not conserved. The result leads to a relationship
that is bounded on the high and low ends with respect to both
target material atomic mass and thickness.
For innitely thick electron targets in directional geometry,
silver shows the greatest efciency of bremsstrahlung conversion
of incident electrons at low energies. At high energies, copper
performs the best. This can be explained by the competing
relationship between bremsstrahlung efciency and X-ray mass
attenuation. Due to its low mass attenuation and low atomic
number copper shows a large absorption at low energies of the
few photons generated. In comparison, silver and molybdenum
Fig. 5
Fig. 6
Fig. 7
Fig. 8
M. Klopfer et al. / Nuclear Instruments and Methods in Physics Research A 689 (2012) 4751 50
outperform copper at these energies due to a greater bremsstrah-
lung despite increased self-attenuation because the conversion
events occur closer to the surface of the material, reducing the
total attenuation. In addition, silver shows enhanced conversion
efciency at 30 keV due to K
a1,b1
shell uorescence peak at 22.96
and 24.94 keV. At higher atomic masses, silver and molybdenum
generate greater numbers of photons through more efcient
bremsstrahlung conversion. The self-attenuation of generated
photons is greater as compared to copper. The other high-z materials
studied, gold and tungsten, have sufcient mass attenuation to
absorb generated photons, and despite their higher bremsstrahlung
conversion efciency, the increased attenuation severely attenuates
generated photons. This results in lower emission efciencies in
comparison to silver and molybdenumacross the entire investigated
energy band.
For transmission geometry, generated photons need to pass
through the target material to be counted as emission. Any X-ray
production that is not directed through the material is assumed to
be lost energy. As in the directional geometry case, self-attenua-
tion of the target material leads to loss of photons. For transmis-
sion geometry, the target material must be thick enough to allow
sufcient conversion of electrons to photons, yet not too thick so
as to attenuate generated photons. This relationship is strongly
dependent on incident electron energy, especially for low energy
electrons. After target thickness values have been determined
for the optimum conversion efciency, similar relationships for
photon production efciency between silver and copper are
observed for high and low energies as in the directional target
simulation.
Thus, from our studies it is seen that the choice of target
material and target thickness for the most efcient X-ray emis-
sion depends on the energy range to be used. These factors have
to be taken into account when designing a particular X-ray
source.
5. Conclusions
Through the course of this study we simulated pyroelectric
X-ray emission for various common electron-target materials and
multiple incident energies to nd maximum electronphoton
conversion efciencies. Reduction of the modeling of the complex
packeted emission properties of pyroelectric sources leads to
simplied device modeling. The results of studies on anode
designs show that the highest efciency of X-ray emission
depends on target material as well as on incident electron energy.
The work presented can be used to guide further design for
experimental and commercial pyroelectric X-ray sources for
industrial and medical applications.
Acknowledgments
The authors would like to thank Dr. James Brownridge and Dr.
Yaron Danon for the insightful discussions that helped us bring
this project to fruition. We would also like to thank Crystal
Technologies for the donation of the crystals used during the
course of these experiments.
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