wide band-gap photovoltaics
TRANSCRIPT
Wide Band-Gap Photovoltaics
M.A. Prelasa, G. Popov1cia,b, Salim Khasawinaha, and Jeff Sunga
a) College of Engineering, University of Missouri, Columbia, MO 65211
b) Rockford Diamond Technology, Professional Arts Bldg., S. 6th Street, suite 101,
Champaign, IL 61801
Abstract
Wide bandgap materials will have many applications as coatings and as electronic devices. This paper describes an electronic application for wide bandgap materials in energy production. A specific portable power technology which converts the energy emitted from nuclear reactions to electrical energy using wide bandgap photovoltaic cells without intermediate thermalization is described in this paper. The potential efficiency for the pho
tovoltaic process is 35%, nuclear energy to electrical energy. And, if combined with hightemperature thermionic conversion the nuclear to electrical energy conversion efficiency is 41% while the overall size of the system remains small. The key to the process is to first convert the high-grade ion energy to photon energy, which can then be directly converted to electrical energy. This process is also usable as an advanced topping cycle for large scale energy production in conjunction with fusion power, as well as fission power. In addition to improved efficiency, the process also promises advantages in smaller volumes,
smaller mass, and lower cost of the energy conversion hardware.
Introduction
The use of wide bandgap photovoltaics (e.g., diamond and aluminum nitride) in fusion
energy conversion was discussed in 1981 [1] and in fission energy conversion was discussed in 1984 [2]. The focus of this discussion will be in the use and implementation of
radioisotopes. In this paper the process of nuclear energy conversion with wide bandgap
photovoltaics will be called the £hotovoltaic £nergy conversion of Nuclear energy fu'stem (PENS). PENS can use both gaseous or solid nuclear fuels for power production. A
summary of how solid fuels can be introduced into PENS is given in References 3 and 4. The important underlying principle is to introduce the solid into the PENS so that it opti-
463
M.A. Prelas et al. (eds.), Wide Band Gap Electronic Materials, 463-474 © 1995 Kluwer Academic Publishers. Printed in the Netherlands.
464
cally thin. This can be achieved by introducing the solid as an aerosol, thin fibers, thin films, or encapsulating the individual atoms ofthe solid in Fullerenes [3,4].
In the first step of the PENS, the nuclear energy is transported to a fluorescer which converts it into photons. (The fluorescer could be a solid, liquid, or gas. This paper will focus on the use of a gas.) Then, in the second step of the process, the photons are transported out of the active region to high bandgap photovoltaic cells which efficiently convert the photon energy
to electricity.
Figure 1. Schematic Diagram of the PENS.
The efficiency of the two-step PENS process, while inherently less efficient than one-step
direct energy conversion has two major advantages over thermal energy conversion, which
is a many step process. These advantages are: 1) that it is a direct process producing a useful energy form from high grade energy and thus avoiding the Carnot cycle efficiency limits imposed by thermalization and 2) that it is much simpler, potentially leading to more com
pact, more reliable, and less expensive energy conversion systems. '
The advantage of the PENS process over a one-step direct energy conversion process is that
of feasibility. The scale length for the transport of the primary high-grade energy must match the geometrical scale of the energy converter. Energetic ions have a transport length
of micrometers while useful energy converters, on the other hand, have a scale length of fractions of meters. For this reason direct conversion of nuclear energy has not previously been possible. What was required was the concept of an intermediate high-level energy converter that can be intermingled with nuclear material on a micrometer scale-length but pro
duces an energy form that can be transported to meter scale-length direct converters
prod1 With
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465
producing useful output- a sort of "impedance matching" for scale length of energy forms.
With PENS that scale length matching medium is a fluorescing gas, the nuclear-driven flu
orescer. The photons it produces can be transported great distances, making it possible to
couple them to various energy conversion processes. Also, some conversion processes re
quire greater power densities than the primary energy sources can provide. A PENS inter
mediate photon flux can be absorbed in a smaller volume than that in which it is produced,
effectively concentrating the flux, enabling achievement of the high threshold power densi
ty for such conversion processes.
Charged Particles
Thin Rectangular Film Thin Cylindrical Fiber
Small Aerosol Particles
Figure 2. An illustration of the use of thin solid geometries which allow reaction products to escape the solid matrix into a surrounding gas.
The RECS concept of high efficiency production of light from radioisotopes makes this
concept useful for remote power applications.
The choice of the fluorescer is important to the process. What is desired is that the fluorescer
emits the energy deposited in it efficiently at a single wavelength without self absorption.
The closest thing to a perfect fluorescer in nature is an excimer or an exciplex. If an atom
(or molecule) is exited (So-> S1*) the atom or molecule can migrate and bond with an un
excited molecule (SoS1 *). If the atoms or molecules are identical then the resulting mole
cule is called and excimer, if the atoms or molecules are different then the resulting
molecule is called an exciplex. The excimer/exciplex rapidly falls apart after the emission
of narrow band fluorescence since the ground state is unbound. Excimers/exciplexes have
been experimentally shown to be efficient (up to 50%), narrow band (+/-10om), non self
absorbing fluorescers [see review in reference 3].
466
Some of the most efficient excimers fluoresce in the vacuum ultraviolet (He2*- 80 nm- 50%
efficient, Ar2*-129 nm- 50% efficient, Kr2*- 147nm- 47% efficient, Xe2*- 172nm- 48% efficient).
Thus, to convert these excimer's narrow band fluorescence to electrical energy requires
wide bandgap photovoltaics. At this time the technology for wide bandgap photovoltaics is not mature. Several promising materials- such as SiC, C (diamond), and AlN- do exist.
Progress has been made in fabricating simple devices such as Schottky barrier diodes on diamond and platinum silicide [5,6], a primitive p-njunction in diamond [7], n-type dia
mond material has been developed [8], and p-type and n-type aluminum nitride have been claimed [9,10]. Progress is being made on the fabrication of wide bandgap photovoltaics.
The use of portable power sources using radioisotopes have been reported [11] and could have immediate applications in space exploration. The current generation oflong lived portable power supplies are based upon the isotope Pu238 which is used to power the Radioisotope Thermion Generator (RTG) for missions such as the Voyager. In the Voyager, three
RTG units produced 7,200 watts of thermal power and 540 watts of electricity regulated to 30 volts from 12,900 grams of the isotope.
Fluorescers
The Ion Source
An example of the PENS is shown in Figure 3 where the ion source is from the decay of
radioisotopes dispersed within a fluorescer gas. Effective dispersal is essential so that the ions produced by the isotope decay deposit most of their kinetic energy in the excimer gas rather than in the radioisotope material. There are at least four methods of achieving the desired dispersal: gaseous radioisotopes, radioisotopes embedded in thin films, radioisotopes
embedded in thin fibers, or microscopic aerosol of radioisotopes. The efficiency of transport of the ion energy from the radioisotope to the fluorescer medium varies with the scale length of the thin film, fibers or aerosol, the chemical form of the radioisotope, and the uniforrnity of the radioisotope density. The variation of ion energy transport efficiency from a
microsphere, to the fluorescer medium, with thin films and microspheres are discussed in
Reference 12. Energy transport efficiencies are about 50% for reasonably designed thin
films, 62% for reasonably designed fibers, and 70% for reasonably designed microspheres. The average atomic density in the medium must be on the order of 1x1019 particles cm-3,
enough to achieve reasonable power densities but not so great as to significantly degrade
the transport of the fluorescence through the aerosol. Combining the constraints of efficiency, and optical transparency determines scale length of the thin film, fibers, or microspheres
and number density. For example, a microsphere diameter of 5 j.!m and number density of
1xl06 cm-3, which should not create significant absorption of the fluorescence [12], results in a fuel density of 0.63 mg cm-3, quite reasonable dimensions, and good number densities
(3.9x1019 atoms cm-3). However, we believe that fibers would be an improvement. As dis-
-80 nm- 50%
'c. efficient).
nr requires .otovoltaics is
~-do exist. er diodes on , n-type dia
ide have been >hotovoltaics.
11] and could long lived por•er the RadioVoyager, three
ty regulated to
n the decay of
1tial so that the the excimer gas lChieving the deIS, radioisotopes
ciency of trans
~s with the scale ope, and the uni
:fficiency from a
are discussed in ' designed thin
ed microspheres. ·9 particles cm-3,
ficantly degrade
traints of efficien;, or microspheres
mmber density of
:ence [12], results
number densities
>rovement. As dis-
467
cussed in Reference 12, a diameter of 5 flm results in an ion transport efficiency of about 60%.
Pressure Vessel
Wide Band Gap Photovoltaics
Figure 3. Schematic Diagram of the PENS which uses a radioisotope fuel in aerosol form.
The structure of a fission fueled PENS is discussed in Reference 12, and a fusion fueled PENS in Reference 13.
Excimer Fluorescers
Excimer fluorescers are the most efficient radiators known and, because of their unbound lower levels, do not self absorb. They radiate in the single, relatively narrow, band of wave
lengths required for efficient photovoltaic energy conversion [12]. The intrinsic fluores
cence efficiencies of rare-gas and rare-gas halide excimers, based on standard W -value
theory [12], are listed in Table 1. Achievable efficiencies should be near the intrinsic values
at the power and electron densities characteristic of nuclear reactions.
In fact one group has reported measuring a nuclear-driven rare-gas excimer fluorescence
efficiency higher than that predicted by W-value theory [12]. Measurements of actual flu
orescence efficiencies at various laboratories, including Lawrence Livermore National
Laboratory, have demonstrated high fluorescence efficiencies for excimers. Experiments with a variety of excitation sources (e.g. electrons, fission fragments, protons) and particle densities have given fluorescence efficiency values ranging from a few percent to as high
as 68% (see review paper by Prelas et al. [12]). The most efficient excimer fluorescers are the rare-gas excimers. Ion-Driven Fluorescers are discussed in much greater detail in the
paper "Nuclear-Driven Flashlamps" [12].
468
Table 1: Theoretical Maximum Intrinsic Photovoltaic, T\pv• and Ion-to-Electric, T\ie• Efficiencies for Selected Rare-Gas and Rare-Gas Halide Excimer Fluorescers with
Matched High-Bandgap Photovoltaic Materials.
Energy Photovoltaic Bandgap
Tti= TtpvX Ttf Ttf Energy Tlpv= EgfEI
Excimer (eV) Material (eV)
Efficiency
Ar2* 0.50 9.6 A1N 6.2 0.65 0.33
Kr2* 0.47 8.4 AlN 6.2 0.74 0.35
Diamond 5.5 0.65 0.31
F2* 0.44 7.8 AlN 6.2 0.79 0.35
Diamond 5.5 0.71 0.31
Xe2* 0.48 7.2 AlN 6.2 0.85 0.41
Diamond 5.5 0.76 0.37
ArF* 0.35 6.4 AlN 6.0 0.94 0.33
Diamond 5.5 0.86 0.30
KrBr* 0.33 6.0 Diamond 5.5 0.92 0.30
KrCl* 0.31 5.6 Diamond 5.5 0.98 0.30
Na2* 0.46 2.84 ZnSe 2.7 0.95 0.44
SiC 2.4 0.845 0.39
Li2* 0.42 2.7 CuA1Se2 2.6 0.96 0.40
SiC 2.4 0.89 0.37
Hg2* 0.21 2.58 GaS 2.5 0.97 0.20
SiC 2.4 0.93 0.19
ArO* 0.11 2.27 GaP 2.2 0.97 0.105
GaAlAs 2.2 0.97 ' 0.105
KrO* 0.13 2.27 GaP 2.2 0.97 0.125
GaA1As 2.2 0.97 0.125
X eO* 0.15 2.27 GaP 2.2 0.97 0.145
GaA1As 2.2 0.97 0.145
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469
The Photon Energy Converter
The key to the feasibility of the PENS is the photovoltaic Photon Energy Converter. The
common impression of photovoltaics is that they cannot be very efficient. This misunder
standing comes from the fact that photovoltaics are most commonly employed as "solar
cells." And solar cells are not very efficient, ranging from 10-20% for commercial units and
reaching as high as about 25% for laboratory cells. However the low efficiency is more due
to the characteristics of the solar spectrum than to the photovoltaics devices themselves, especially for the laboratory units with efficiencies of -25%. The problem with the solar spectrum is that it is very broadband - its ratio of the average photon energy to the width
(FWHM) of the spectrum (Emeanl ~E) is about 1. This is good for color vision but quite bad
for efficient energy conversion.For excimers, however, this ratio is greater than 10. Under
these conditions photovoltaics have intrinsic efficiencies of75-95%.
Photovoltaic cells for use in photon-intermediate direct energy conversion of electricity
will require the development of a doped semiconductor material with a bandgap that matches the UV radiation. With such photovoltaic cells, a system efficiency of 56% for fusion ion
driven fluorescence has been projected [13]. Studies of fission ion driven fluorescence in
dicate that system efficiencies of about 40% are possible [12].
Photovoltaic Conversion of Narrowband Fluorescence
For Xe2 *, E,eanl ~ = 14,compared to a corresponding value of 1.3 for the AM2 solar spec
trum. For a narrow distribution one can have E/Emean -1 and still have 11E0 -1. A narrowband
spectrum will consequently have the highest intrinsic efficiency.
For a given spectrum, the efficiency of conversion is basically determined by the variation
of the irradiance with photon energy and by the substrate bandgap energy, Eg, of the pho
tovoltaic converter. Complete conversion (100%) is not possible because of the width of
the solar spectrum. This leads to two competing effects on the efficiency. The first effect is
that the energy of all photons with quantum energy hv<E8 is lost because they do not have
sufficient energy to excite electrons from the valence band to the conduction band. The
power density lost in this case is given by
Es
plost = JW(E)dE 0
(eq. 1)
where W(E) is the irradiance in W/cm2/eV. Thus, the lower the bandgap of the photovoltaic
converter, the larger the fraction of the total spectrum converted. Competing with this effect
however is the fact that, for the photons with quantum energy hv>E8 that do contribute, the
photon energy in excess of the bandgap energy is lost. Thus the maximum intrinsic efficien-
470
cy for photovoltaic conversion is assuming an ideal collection device is given in equation 2.
- E J (W(E) ;dE) E
(eq. 2} 'TI;n = -L------
JW(E)dE E,
Typically the effect of the details of the solar radiation spectrum on calculating overall con
version efficiency is translated into a photon flux density, which then relates to an ideal
short circuit current density. This is convenient because it is a good assumption that each
photon absorbed and collected effectively causes one electron to move around the circuit.
Also after each electron thermalizes, that is, gives off energy in excess of Eg to the lattice, it contributes maximally a constant Eg in energy to the overall process [13].
Figure 4. The theoretical maximum conversion efficiency of photovoltaic cells with various bandgap energies using either a solar spectrum or a Xe2* spectrum. Bandgap energies associated with Si, GaAs, diamond, and AlN are shown [13].
This contribution is conveniently modeled in the photovoltaic device using the ideal Shock-
ley model
be written
1l
whereNp1
valE>Eg,
Figure4i
ergy ofth trumand,
these coo
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Radiatio1
1uation 2.
rerallcon
an ideal ~hat each
te circuit.
1e lattice,
with varilm. Bandt [13].
eal Shock-
471
ley model for the p-njunction. Using these concepts the intrinsic conversion efficiency can be written in the following terms [13],
EgJNph(E)dE Eg N(E>Eg) = E - N
n = 8 - E tot 'lin J N (E) EdE mean ph
Es
Eg ~11eg
mean (eq. 3)
where ~ph is the photon flux density, in #/s-cm2-eV, N(E>E8) is the photon flux in the interval E>E8 , N101 is the total photon flux, and 1'\eg is the fraction of photons with E>E8 •
Figure 4 is a plot of maximum efficiencies for a p-n junction converter versus bandgap energy of the converter substrate material. Two plots are shown, one for an AM2 solar spec
trum and one for a Xe2* spectrum. The previously derived equations were used to calculate these curves. Also shown are vertical lines representing the bandgap energies of the two materials theoretically predicted to maximally convert these two spectra. Lines representing Si and diamond are shown for comparison. The approximately 30% maximum is thought to be an upper bound on the ability of a single material junction to convert the solar spectrum. The highest known conversion efficiency for silicon, to date, has been 26% obtained with a highly optimized MIS solar cell.
In contrast to the relatively low values for conversion of the solar spectrum, it can be seen from Figure 4 that efficiencies as high as 80% can theoretically be obtained using a p-n junction and converting the Xe2 • spectrum. Although it is still speculative about whether or not high quality p-njunctions can be made in materials with bandgaps above 4 eV, it is encouraging to note that high conversion efficiencies are possible.
Wide Bandgap Photovoltaic Materials
Table 1 lists several potential wide bandgap materials. Table 1 matches the more efficient
and desirable fluorescers to materials with appropriate band gaps. The theoretical maximum
intrinsic photovoltaic efficiency (the ratio of the bandgap to the mean photon energy ranges
from 75% to 95%) while the corresponding theoretical maximum efficiency for conversion
of ion energy to electrical energy (the product of the photo voltaic efficiency and the fluo
rescence efficiency) ranges from 30% to 45%. If the most optimistic reported values of the fluorescence efficiency were used, the maximum ion-to-electric efficiency would increase to 56%. The outlook for such cells is hopeful [11]. Rare-gas halide excimers have lower
photon energies (3.5 eV for XeF*, 5.0 eV for KrF*, and 6.4 eV for ArF*) and, while their fluorescence efficiency may be lower than that of the rare-gas excimers, their photon ener
gy falls in the range of well known semiconductor materials.
Radiation damage to the photovoltaics from X-rays and neutrons is a concern. However, it
472
is well known that ionizing radiation appears to enhance fluorescence absorption efficiency
in continuous-wave insulating crystal lasers. Additionally, if a radiation damaged crystal is
thermally annealed, the damage disappears. Potential crystalline photovoltaic materials
which may experience the positive effects described above exist (Diamond and Aluminum
Nitride).
Integration of Ion Source to Photovoltaics
Ion Source
There are many potential ion sources which can be used for the conversion method. For example, it is possible to use fission reactions (e.g., u233(n,ff1)ffh, u235(n,ff1)ffh, or Pu239(n,
ff1)ffh), fusion reactions (when such sources become feasible), or radioisotopes (e.g, A~9• ~5, s~o. Po210, Pu238, etc.). We have chosen in this discussion to focus on the use of ra
dioisotopes for scaling estimates (see Figure 5).
In these studies the parameter which influenced the systems scale and power source life
time was the radioisotope halflife (Kr85-10.76 yrs, s~0-29 yrs, Po210-0.38 yrs, and Pu238-
87.74 yrs).
Both the scale size and the gamma ray emitted from the reaction influenced the system's
mass. We were conservative in our estimate of a personnel radiation shield by requiring that
the contact radiation be less than 2.5 millirems per hour (e.g., Kr85 -0.514 MeV y 0.38% of
decays, S~0-no y, Po210-0.802 MeV y0.0011% of decays, and Pu238-0.567 MeV y 5x10-5% of decays).
Coupling of Ion Energy to the Fluorescence Source
Based upon the above criteria, we believe that compact power sources can be made from
radioisotopes. The radioisotope ion source can be gaseous (e.g., Kr85 with a half life of
10.76 years which emits a 0.67 MeV beta 100% ofthe decays and a 0.514 MeV gamma
0.38% of the decays), or it can be in the form of a solid (e.g., a thin film, embedded in a
fiber, or as an aerosol--See Figure 1). The types of solid radioisotopes which can be used
in the mobile power system are: S~0 with a half life of 29 years which emits only a 0.67
MeV beta; Po210 with a halflife of 138.4 days which emits a 5.305 MeV alpha 100% of the
decays and a 0.803 MeV gamma 0.0011% of the decays; and Pu238 with a half life of 86.4
years which emits a 5.5 MeV alpha 100% of the decays and a 0.77 MeV gamma 1x10-5%
of the decays. The Pu238 source was used to power the RTG used in the Voyager spacecraft.
Three RTG units produced 7200 watts of thermal power and 540 watts of electricity regu
lated to 30 volts from 12,900 grams of the isotope. Using the PENS concept, 12,900 grams
of Pu238 could produce 2,616 Watts of electrical power.
0
2
0
8
6
50
25
00
75
75
so
25
00
75
FigureS.
fficiency ~rystal is
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em
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0
473
Figure 5. Estimation of PENS mass, scale, and decay are shown for Kr85, s~0• Po210, and Pu238. The geometry is assumed to be spherical with a diameter equal to the system scale estimation. Photovoltaic cells are assumed to surround the fluorescer media and the vessel is shielded with lead.
474
Making an integrated system which produces a significant power density and remains op
tically thin is a challenge. The use of thin films, fibers, or aerosols along with thin aluminum or silver coatings have been examined in Prelas, Boody, Kunze, and Miley 1988. With solid materials, an average atomic density of approximately 5x1019 atoms cm-3 can be
achieved for a reasonably optically thin system. The optical transport properties of films, fibers, or aerosols can be enhanced by a thin coating of reflective material [12]. Charged particles can penetrate the thin reflective coating without losing significant energy or significantly effecting the coating [12].
References
1) M.A. Prelas, "A Potential UV Fusion Light bulb for Energy Conversion", Bult. of the Am. Phys. Soc., 26(1), 1045, 1981: See also Inside R&D, Vol. 10, Number 41 (Oct. 14, 1981).
2) M. A. Prelas, F. P. Boody, M. Zediker and M. Rowe, "A Direct Energy Conversion Technique Based on an Aerosol Core Reactor Concept", 1984 IEEE Int. Conf. on Plasma Sci., IEEE Publication Number: 84CH1958-8, 38, 1984.
3) M.A. Prelas, E. J. Charlson, F. P. Boody, and G. H. Miley, Prog. In Nuclear Energy, 23 (3), pp. 223-240 (1990).
4) D. J. Mencin and M.A. Prelas, "Low Temperature Gaseous Core Reactors Using Uranium Particles Trapped in C60 Cages," Proceedings of Nuclear Technologies for Space Exploration," Sponsored by the Idaho Section of the American Nuclear Society, Snow King Resort, Jackson Hole Wyoming, August 16-19, 1992.
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7) T. Stacy, et. al., "Rectifying Contact Formation with Indium on Polycrystalline p-type Hot Filament CVD Diamond Utilizing Molecular Ion Implantation," Accepted for Publication in Journal of Applied Physics (February, 1993).
8) Galina Popovici, T. Sung, M. Prelas, and S. Khasawinah, "Evidence for n-type Diamond," Gordon Conference on Diamond Films, June 1994.
9) W. M Yirn, E. J. Stofko, P. J. Zanzucchi, J. I. Pankove, M. Ettenberg, and S. L. Bilbert, J. Appl. Phys., 44, 29 (1973)
10) R. F. Davis, Proc. IEEE, 79, No.5, 702 (1991).
11) M. Prelas, E. J. Charlson, E. M. Charlson, J. Meese, G. Popovici, and T. ~tacy, "Diamond Photovoltaic in Energy Conversion," Second International Conference on the Applications of Diamond Films and Related Materials, M. Yoshikawa, M. Murakawa, Y. Tzeng and W. A. Yarbrough editors, MYU, Tokyo (ISBN 4-943995-07-1), 329-334 (1993)
12) M.A. Prelas, F. P. Boody, G. H. Miley, and J. Kunze, "Nuclear-Driven Flashlamps", Lasers and Particle Beams, 6(1), 25, 1988; also, M.A. Prelas, and S. Loyalka, Progress in Nuclear Energy, 8, 35-52, 1981
13) M.A. Prelas, E. J. Charlson, E. M. Charlson, J. Meese, G. Popovici, and T. Stacy, "Diamond and Diamond Like Substrates as First Wall Materials in Inertial Confinement Fusion," Lasers and Particle Beams, 11(1), 65-79 (1993).
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