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Rajagopal, Adharsh
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article
Enhancing Defect Tolerance and Phase Stability of High-Bandgap Perovskites via Guanidinium Alloying
Abstract
The open-circuit voltages (V<sub>OC</sub>) of hybrid perovskite (HP) solar cells do not increase sufficiently with increasing bandgap (for Eg > 1.70eV). We study the impact of A<sup>+</sup> size mismatch induced lattice distortions (in ABX<sub>3</sub> 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<sub>0.33</sub>GA<sub>0.19</sub>Cs<sub>0.47</sub>)Pb(I<sub>0.66</sub>Br<sub>0.34</sub>)<sub>3</sub> and 1.75eV bandgap (FA<sub>0.58</sub>GA<sub>0.10</sub>Cs<sub>0.32</sub>)Pb(I<sub>0.73</sub>Br<sub>0.27</sub>)<sub>3</sub> 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)<sub>3</sub> are then used to fabricate p-i-n photovoltaic devices that have a V<sub>OC</sub> of 1.24 V. This V<sub>OC</sub> is among the highest V<sub>OC</sub> 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)<sub>3</sub> films and prove that FA-GA-Cs alloying is a viable route to attain high V<sub>OC</sub> in high-bandgap HP solar cells.