Journal
ACS ENERGY LETTERS
Volume 3, Issue 6, Pages 1261-1268Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.8b00576
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Funding
- U.S. Department of Energy SunShot Initiative
- Next Generation Photovoltaics 3 program
- Office of Naval Research [ONR N00014-17-1-2260]
- State of Washington through the University of Washington Clean Energy Institute
- Washington Research Foundation
- [DE-EE0006710]
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The open-circuit voltages (V-OC) of hybrid perovskite (HP) solar cells do not increase sufficiently with increasing bandgap (for Eg > 1.70eV). We study the impact of A(+) size mismatch induced lattice distortions (in ABX(3) structure) on the optoelectronic quality of high-bandgap HPs and find that the highest quality films have high A-site size-mismatch, where large guanidinium (GA) compensates for small Cs to keep the tolerance factor in the range for the perovskite structure. Specifically, we find that 1.84eV bandgap (FA(0.33)GA(0.19)Cs(0.47))Pb (I(0.66)Bro(0.34))(3) and 1.75eV bandgap (FA(0.58)GA(0.10)Cs(0.32))Pb(I(0.73)Bro(0.27))(3) attain quasi-Fermi level splitting of 1.43eV and 1.35eV, respectively, which is >91% of the Shockley-Queisser limit for both cases. Films of 1.75eV bandgap (FA,GA,Cs)Pb(I,Br)(3) are then used to fabricate p-i-n photovoltaic devices that have a V-OC of 1.24 V. This V-OC is among the highest V-OC reported for any HPs with similar bandgap (1.7 to 1.8 eV) and a substantial improvement for the p-i-n architecture, which is desirable for tandems with Si, CIGS, or a low-bandgap HP. Collectively, our results show that non-radiative recombination rates are reduced in (FA,GA,Cs)Pb(I,Br)(3) films and prove that FA-GA-Cs alloying is a viable route to attain high V-OC in high-bandgap HP solar cells.
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