High efficiency 4H-SiC Betavoltaic Power Sources using Tritium
Radioisotopes
Supplemental Information
Christopher Thomas1, Samuel Portnoff 1, and M. G. Spencer2
1
2
Widetronix Corp, Ithaca, New York, 14850 USA
Dept. of Electrical and Computer Engineering, Cornell University, Ithaca, New York, 14850 USA
A. Calculation of Beta Spectrum
The Fermi approximation is used to calculate the beta spectrum1
4π
(S1) ππ½ (π)ππ = 137
π
4π
1
(π 2 β1)2
{1 β ππ₯π (β 137
π
1
(π 2 β1)2
)} ((π 2 β 1))π(ππππ₯ β π)2 ππ
where π =kinetic + rest energy of emitted beta particle and ππππ₯ =max kinetic energy +rest
energy of the emitted beta particle (in units of rest energy). Substituting πΈ β² for π β² where πΈ β² =1+ π
/moec2 and moe is the mass of an electron πΈ β² πππ₯ =1+ π max/ moec2
2
(S2) ππ½ (ππ½ )πππ½ = πΆπ π(π, πΈ β² )(πΈ β² β 1)πΈ β² (πΈ β² πππ₯ β πΈ β² )2 πππ½
where f is the Fermi function. The coefficient CN is calculated so that the distribution function is
normalized
π
(S3) 1 = β«0 π½πππ₯ ππ½ (ππ½ )πππ½
The average value of energy is calculated by
πΈ β² πππ₯
(S4) β©πΈ β² β 1βͺπ΄π£π = β«1
(πΈ β² β 1)ππ½ (ππ½ )πππ½
Fig S1 (left) shows the calculated beta spectrum for 1ML of TiH32 while (right) shows the beta
spectrum for .4 microns of TiH32 note the shift in the position of the maximum energy when
multiple monolayers are used. This shift is due to self-absorption and will be discussed in B.
1
1.5 10
-3
Probability (arb. units)
Beta Distribution for
one ML Hydride Thickness
1 10
-3
5 10
-4
Beta Distribution
Hydride Thickness .4u
0
0
5
10
15
20
Beta Energy (keV)
Figure S1 Calculated beta distribution function for one monolayer of TiH 32 and for TiH32 of thickness .4 microns
B. Calculation of Self Absorption in TiH32
The maximum absorption range of electrons in TiH32 and SiC was calculated using the
relationship given by Everhart 2
4
(S5) π
(πΈ) = πΈ01.75 100π
where R(E) is the range in microns, E0 is the incident energy of the electron in keV and π is the
density of the TiH32 in g/cm3 . The empirical equations of Kanaya and Okayama3 were used to
calculate the beta energy spectrum from a TiH32 of thickness d. The TiH32 was divided in to n
monolayers
(S6) π = ππΏ
π
πβππππππ π
Where MLThickness is the thickness of one monolayer of TiH32. Individual electrons will transverse
a distance equal to ML*n. For incident energies in the beta spectrum a Matlab program was used
to calculate the reduced energy of the electrons originating from the nth monolayer at the edge of
the foil (S6). These electrons can be either reflected, absorbed or transmitted using (S7) to
calculate the transmission percentage at the edge of the TiH32.
2
(S7) πΈπ = (1 β π¦)2/3 πΈ0
where y is the reduced depth x/R(E0) and E0 is the starting energy of the electron from the nth
monolayer
πΎπ¦
(S8) ππ = exp(β 1βπ¦)
2
Where πΎ = .187π 3
and Z is the atomic number of the absorbing material
Fig S2 shows the calculated beta spectrum for several thickness of TiH32 100% conversion of the
titanium is assumed. The average beta energies and total particle flux are computed for each
thickness, notice the shift of average energy to higher values as the thickness increases due to
absorption of the lower energy betas. Also note the saturation in particle flux for thickness
greater than .4um. The saturation in particle flux is because .4um is approximately the maximum
range for tritium betas
8.5
7 108
7.5
6 10
8
5 10
8
4 10
8
-2
Beta Flux (cm )
Avg Beta Energy (keV)
8
7
6.5
3 108
2 108
6
1 10
5.5
8
0
0
0.1
0.2
0.3
0.4
0.5
0.6
Titanium Hydride Thickness (microns)
0
0.1
0.2
0.3
0.4
0.5
0.6
Titanium Hydride Thickness (Microns)
Figure S2a,b (left) Average energy of electrons leaving foil of TiH32as a function of foil thickness. (right)
Flux of electrons leaving foil of TiH32 as a function of foil thickness
C. Measurement of Input Power
The input power is calculated from (S9)
(S9) πππππ’π‘ = π½π½ β©ππ½ βͺ where π½π½ is the beta flux.
3
The beta flux is measured using a surface activity monitor adapted from Liu4 . The measured
data from an example foil is plotted in Fig 3. The voltage on the plates is increased until current
saturation occurs. The current at saturation is given by (S10)
(S10) π½ππππ π’πππ = π½π½ππ‘π π
β©ππ½ βͺ
πππππ ππ‘πππ πππ
where the ionization of air occurs at
ionization
air=33.7eV
Based on these measurements, the saturation current (at 100V) is 7.83na. The area of the foil is
.36cm-2. Pinput is calculated as 732.9nW cm-2. Using a average energy of 8.25keV the beta flux
produced is 5.54x108 cm-2 which correspond to a specific activity of 14.97 mCi. This foil
produced 85% of the max beta flux calculated in B.
Ionization Current (Amps)
1 10
-8
8 10-9
6 10-9
4 10-9
2 10-9
0
0
50
100
150
200
250
Voltage (V)
Figure S3 Air ionization current as a function of applied voltage between electrodes forming an air
gap. Test sample is placed on bottom electrode
D. Correction of Power due to Absorption in Palladium layer
The schematic of our TiH32 layer is shown in Fig 2. I n the main text. Equal numbers of beta
electrons are emitted up as down. However the electrons travelling in an upward direction have
an extra absorption due to the presence of a 20nm thick Pd layer. In our calculation of efficiency
this will cause an underestimation of the electrons traveling in the downward direction. Using
4
the simulation developed in B we calculation the ratio of the output power from electrons
traveling up/ electrons traveling down. The calculated value was .62 this value is used to correct
the efficiency calculation.
E. Calculation of the beta backscattering percentage
The backscatter correction to the calculation of betavoltaic conversion efficiency given by (S11)
(S11)
β©πΈπ΅ βͺ
π = ππ΅ β©πΈ
ππππ βͺ
Where ππ΅ is the percentage of the total electrons backscattered. Experimentally it has been
determined that the backscattering electron energy is significantly less than the incoming energy.
β©πΈπ΅ βͺ
Therefore the backscattering correction term is given by ππ΅ β©πΈ
ππππ βͺ
β©πΈπ΅ βͺ
backscattering β©πΈ
The mean energy loss from
has experimentally been found to be ~.6 for a Z number of 20. From K&
ππππ βͺ
S3 the total backscatter percentage is given by (S12)
6
π¦
(S12) ππ΅ = 5 β«0
πΎπ΅
πΎπ΅ π¦
exp (β 1βπ¦
) ππ¦
(1βπ¦)7/6
6
πΎ π¦
π΅
β 5π₯25/6 {1 β exp (β 1βπ¦
)}
When (S12) is evaluated at y=1 (the maximum range of the incident electron)
=
6
6
πΎπ΅ exp(βπΎπ΅ ) . 6435 β
5
5π₯25/6
Where πΎπ΅ = 1.9πΎ Table I shows parameters used for the calculation of π
Material
Z#
πΈπ©
πΌπ©
πΌ
SiC
20
2.61
.26
.16
Table SI Parameters used for calculation of electron backscatter correction
F. Calculation of Generation Function
Using the beta spectrum found form the TiH32 as input we calculate the electron hole pair
generation as a function of distance using (S13)
5
π
1
(S13) πΊ(π₯ β² ) = β0π½πππ₯ π(ππ½ ) 7.28ππ
where
ππΈπ΄ (π₯)
ππ₯
ππΈπ΄ (π₯)
ππ₯
|
π₯=π₯ β²
ππ₯
is the change in energy of the electron due to absorption evaluated at xβ and 7.28eV
is the mean ionization energy in SiC 5 and π(ππ½ ) is the spectral function calculated from B.
From the K&S equations
(S14)
ππΈπ΄ (π₯)
ππ₯
=
ππΈ0
π
ππΈπ΄ (π₯)
ππ₯
is given by (S14)
1
πΎπ¦
πΎ
3
{(1βπ¦)2/5 ππ₯π (β 1βπ¦) (1βπ¦ + 5) + πΈπ΅
6π₯1.9
5
πΎ
1.9πΎπ¦
ππ₯π (β 1βπ¦ ) β
(1βπ¦)2
1
(25/6 β (1 β π¦)5/6 )}
The generation function is shown as Fig. S4 in the text
G Calculation of the steady state carrier concentration and short circuit current density
The steady minority carrier concentration and short circuit current density were calculated by
solving the continuity equation for the region of the device between the edge of the depleted
surface (xsurface
depl)
and the edge of the P+N junction depletion region (xd) for calculation
convenience we set x surface depletion =0. For a PN junction in steady state neglecting drift
transport the continuity equation for the top surface is given by (S15)
(S15) π·π
π(ππ βππ0 )
ππ₯ 2
+ πΊ(π₯) β
(ππ βππ0 )
ππ
=0
Where Dn is the diffusion constant for electrons and ππ is the minority carrier lifetime and G(x)
is the generation function calculated in F. We approximate G(x) with a Gaussian distribution
and (S15) in terms of constants A, C, D, a, and b becomes (S16)
(S16) π΄
π(ππ βππ0 )
ππ₯ 2
+ πΆππ₯π (β
(πβπ₯)2
π
) β π·(ππ β ππ0 )
The close form solution is (S17) (π17) (ππ β ππ0 ) = ββπβππΆππ₯π (
βπ·π₯
βπ΄
) erf(
πβπ·β2βπ΄(πβπ₯)
2βπ΄βπ
1
) 4βπ΄βπ· β βπβππΆππ₯π (
πβπ·
βπ΄
ππ·
+ 4π΄ β
βπ·π₯
βπ΄
) erf(
πβπ·
βπ΄
ππ·
+ 4π΄ +
2βπ΄(πβπ₯)+πβπ·
2βπ΄βπ
1
) 4βπ΄βπ·
6
The equation is solved subject to the boundary conditions (S18) and (S19)
(S18) ππ = 0 at x=xd
(S19) π·π
π(ππ βππ0 )
= ππ
ππ₯
Where Sn is the effective surface recombination velocity for electrons The simulation calculates
Jn the junction current, JSrec the recombination current flowing to the surface and JBulk the current
due to recombination in the bulk
(S20) π½π = ππ·π
π(ππ βππ0 )
ππ₯
|
π₯=π₯π
π½ππ
ππ = πππ (ππ β ππ0 )
Results of the calculations for Sn =107 cm/sec for a junction thickness of 2um (left) and .2um
(right) are shown in Fig S4. For Sn=.1 cm/sec
and junction thickness of 2um and using a
minority carrier lifetime of .5-1usec JBulk is not significant. Therefore the maximum junction
current JnMax was set equal to Jn calculated for a junction thickness of 2um (insuring total beta
absorption) and Sn=.1 cm/sec. For junction thicknesses less than 2um and Sn=.1 cm/sec the
difference JnMax - Jn was assumed to be due to absorption of betaβs in the junction depletion
region or the N region. Fig S5 in the text was calculated by (S21)
(S21)
πΆπππ =
π½ππππ₯
π½π
7
1.5 10
6
2.5 105
-3
Minority Carrier Density (cm )
-3
6
Minority Carrier Concentration (cm )
2 10
1 10
5 10
6
5
2 105
1.5 10
5
1 105
5 10
4
0
0
0
0.5
1
Thickness (microns)
1.5
0
0.05
0.1
0.15
Thickness (microns)
Figure S4 Minority carrier density vs top layer junction thickness (junction depletion
edge-surface depletion edge) for a minority carrier lifetime of .5usec and surface
recombination velocity of 107 cm/sec. (left) junction thickness of 2um (right) junction
thickness of .2um
References
S1. Polymers, Phosphors and Voltaics for Radioisotope Microbatteries edited by Kenneth E.
Bower, Yuri A. Barbanel , Yuri G. Shreter, and George W. Bohnert Chap 2 p55 and
references therein
S2. Everhart, TE, Hoff, PH Journal of Applied Physics 42 pp. 5837-5846 (1971)
S3. Kanaya, K and Okayama, S Journal of Physics D 5 pp. 43-58 (1972)
S4. Liu, Baojun, Chen, KP, Kherani, NP, Zukotynski, S, Antoniazzi, AB Applied Physics
Letters 92 083511 (2008)
S5. Sandeep K Chaudhuri, Kelvin, J. Zavalla and Krishna C. Mandal, Applied Physics
Letters 102, 03119 (2013)
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