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Supporting Information

Potential of High Stability Perovskite Solar Cells for Low-Intensity-Low-


Temperature (LILT) Outer Planetary Space Missions

C. R. Brown1, G. E. Eperon2,3#, V. R. Whiteside1, I. R. Sellers*,1

1 Homer L. Dodge Department of Physics & Astronomy, University of Oklahoma, 440 W. Brooks Street,
Norman, OK 73019, United States
2 Cavendish Laboratory, JJ Thomson Avenue, Cambridge CB3 0HE, UK
3Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, United States
# Present address: National Renewable Energy Laboratory, Golden, Colorado 80401, United States

(*) Correspondence should be addressed to Ian R. Sellers (sellers@ou.edu)

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Materials
Methylammonium iodide, methylammonium bromide, formamidinium iodide and FK209 were
purchased from Greatcell solar. Lead iodide and SnO2 (Tin(IV) oxide, 15% in H2O colloidal
dispersion) were purchased from Alfa Aesar. Spiro-OMeTAD was purchased from Lumtec. All
other chemicals were purchased from Sigma Aldrich. All solvents used are anhydrous.

Solar Cell Fabrication


Triple cation perovskite solar cells were fabricated in the n-i-p architecture, with electron and
hole selective contacts of SnO2 and Li-doped spiro-OMeTAD, respectively (spiro-
OMeTAD= 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamino)-9,9′spirobifluorene). MoOx/Al
was used as a stable metal contact1.
Solar cells were fabricated on ITO-coated glass that had been cleaned with acetone, propan-2-ol
and UV ozone treatment. SnO2 was deposited by spin-coating a solution of 2.67 wt% tin oxide
colloid solution (diluted from 15 wt% commercial solution) in water at 3000 rpm for 30 s,
followed by annealing at 150 oC for 10 mins.
The perovskite precursor solution was dissolved in 1:4 dimethylsulfoxide:dimethylformamide,
with a nominal composition in the precursor solution of (FA0.79MA0.16Cs0.05)0.97Pb(I0.84Br0.16)2.97,
where FA is formamidinium, MA is methylammonium. This was made by dissolving 172 mg
FAI, 507 mg PbI2, 22 mg MABr, 73 mg PbBr2 and 40 μl of CsI stock (1.5 M in DMSO) in the
DMF:DMSO solvent to give a 1.2 M solution (with respect to FA). To form perovskite films,
this was spin-coated at 1000 rpm for 10 s followed by 6000 rpm for 45 s, with 100 uL of anisole
dripped onto the spinning film with 25 seconds remaining in the spin routine. Films were then
annealed at 100 oC for 60 minutes.
Doped spiro-OMeTAD solution was made by dissolving 72 mg spiro-OMeTAD, 29 µl tert-
butylpyridine, 17.5 µl of Li-TFSI stock (520 mg/ml in acetonitrile), 29 µl of FK209 (tris(2-(1H-
pyrazol-1-yl)-4-tert-butylpyridine)cobalt(III)-tris(bis(trifluoromethylsulfonyl)imide) stock (300
mg/ml in acetonitrile) in 1ml chlorobenzene. This solution was spin-coated at 5000 rpm for 30 s
to form the spiro-OMeTAD layer.
15 nm of MoOx followed by 100 nm of Al was thermally evaporated to complete the devices.
The approximate thicknesses of the constituent layers in the solar cell structure are: SnO2 5-20
nm; perovskite ~350-450 nm; Spiro-OMeTAD ~ 100 nm; MoOx 15 nm; and Al 100 nm.

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Characterization
Current-Voltage data were recorded via a Keithley 2400 source meter at AM0, where the
intensity was adjusted using a set of fine mesh grids and the spectrum is adjusted using a AM0
filter #81311 from Newport, a system developed by Scheiman et al. to retain illumination
intensity uniformity and spectral characteristics under LILT conditions2. This methodology
produces a class A spectral match (IEC 60904-9 2007) to the AM0 spectrum from 400-1100 nm,
which is well matched to the absorption of the perovskite solar cells studied here. To verify to
the reduced concentration factor produced, a calibrated silicon reference cell was used.
Temperature control was provided by a custom vacuum compatible Linkam cryostat capable of
temperatures from 77 K to 723 K. To define the exact sample area an aperture was implemented
to ensure accurate current density. Bias-dependent external quantum efficiency (EQE) was
acquired via a custom-built current preamplifier based on a Stanford Research Systems SR555,
and the chopped signal was detected with a Stanford Research Systems SR830 Lock-In
amplifier. A quartz halogen lamp dispersed through a monochromator was used as the light
source, and the reference spectrum was detected using calibrated silicon and germanium
photodiodes. Simultaneous bias dependent photoluminescence and monochromatic J-V
measurements were performed using HeNe excitation at 632.8 nm defocused to match the device
area of ~ 2 mm2 and variable temperature dependent photoluminescence (VT PL) measured in a
Janis closed cycle cryostat, dispersed using a Princeton Instruments spectrometer, and detected
with a silicon CCD.

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Figure S1.
(a) Variable temperature dependent photoluminescence (PL) data. (b) Variable temperature
dependence of PL intensity. (c) Arrhenius plot using the natural log of integrated intensity for the
extraction of activation energy. (d) Variable temperature dependence of the position of the PL
peak expressed in energy.

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Figure S2.
Tauc plot for extracting the band gap from EQE data. Plots are made for each temperature, and
the band gap extracted from the x-intercept of the linear fit.

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Figure S3.
Variable temperature dependent external quantum efficiency (EQE) data at Jsc (0 V).

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Figure S4.
Variable temperature dependent current-voltage data taken under AM0 illumination, in the
reverse direction (from positive to negative bias).

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Table S1.
Table of extracted solar cells parameters before shipment to the University of Oklahoma.
Parameters were extracted from current-voltage scans in the reverse direction.

Voc (V) Jsc Pmp Vmp (V) Jmp FF (%) PCE


(mA/cm2) (mW/cm2) (mA/cm2) (%)
B4_A_01 1.02 21.95 15.64 0.79 19.79 69.50 15.64
B4_C_01 1.02 21.37 14.41 0.80 18.01 66.04 14.41
B4_D_01 1.04 21.93 16.66 0.84 19.83 72.70 16.66
B4_E_01 1.04 21.84 16.54 0.83 19.93 72.59 16.54
B4_F_01 1.03 21.62 15.82 0.81 19.53 71.02 15.82
B10_A_01 1.00 22.05 15.06 0.77 19.56 68.40 15.06
B10_C_01 1.00 21.74 14.86 0.77 19.31 68.14 14.86
B10_D_01 1.00 22.05 15.37 0.78 19.71 69.71 15.37
B10_E_01 1.02 21.85 15.49 0.79 19.61 69.73 15.49
B10_F_01 1.01 21.45 14.73 0.78 18.88 67.76 14.73
B15_A_01 1.02 21.93 15.57 0.80 19.46 69.47 15.57
B15_C_01 1.05 21.59 16.41 0.85 19.31 72.42 16.41
B15_D_01 1.03 21.90 15.92 0.81 19.66 70.59 15.92
B15_E_01 1.03 21.76 16.03 0.82 19.55 71.79 16.03
B15_F_01 1.03 21.70 15.72 0.81 19.41 70.19 15.72
B18_A_01 0.99 21.97 14.76 0.73 20.22 67.79 14.76
B18_C_01 0.98 20.51 12.41 0.73 17.00 61.79 12.41
B18_D_01 0.98 21.97 14.61 0.75 19.48 67.93 14.61
B18_E_01 0.99 21.81 15.27 0.77 19.83 70.70 15.27
B18_F_01 1.00 21.74 15.58 0.79 19.72 71.73 15.58

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Table S2.
Parameters extracted from fitting to perovskite solar cell current-voltage data taken under LILT
conditions at the University of Oklahoma.

Temp Intensity Voc (V) Jsc Pmp Vmp Jmp FF PCE


(K) (% of 1 (mA/cm2) (mW/cm2) (V) (mA/cm2) (%) (%)
Sun AM0)
B4A_300_F 300 100 0.95 22.47 11.83 0.64 18.49 55.54 8.69
B4A_300_R 300 100 1.05 22.61 15.92 0.80 19.95 66.95 11.70
B4A_263_F 263 43.1 0.83 10.07 5.41 0.60 8.98 64.39 9.22
B4A_263_R 263 43.1 1.01 10.09 7.38 0.80 9.22 72.07 12.57
B4A_135_F 135 3.7 0.85 0.89 0.57 0.68 0.84 74.74 11.22
B4A_135_R 135 3.7 0.85 0.89 0.56 0.67 0.84 74.55 11.21
B4A_100_F 100 1.1 0.84 0.26 0.17 0.69 0.24 77.71 11.13
B4A_100_R 100 1.1 0.84 0.26 0.17 0.69 0.24 77.38 11.08

References

1. Christians, J. A.; Schulz, P.; Tinkham, J. S.; Schloemer, T. H.; Harvey, S. P.; Tremolet de
Villers, B. J.; Sellinger, A.; Berry, J. J.; Luther, J. M., Tailored interfaces of unencapsulated
perovskite solar cells for >1,000 hour operational stability. Nature Energy 2018, 3, 68-74.
2. Scheiman, D. A.; Snyder, D. B. In Low intensity low temperature (LILT) measurements
of state-of-the-art triple junction solar cells for space missions, 2008 33rd IEEE Photovoltaic
Specialists Conference, 11-16 May 2008; 2008; pp 1-6.

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