Reducing Surface Recombination Velocity of Methylammonium-Free Mixed-Cation Mixed-Halide Perovskites via Surface Passivation

Jariwala, Sarthak; Burke, Sven; Dunfield, Sean; Shallcross, R. Clayton; Taddei, Margherita; Wang, Jian; Eperon, Giles E.; Armstrong, Neal R.; Berry, Joseph J.; Ginger, David S.

doi:10.1021/acs.chemmater.1c00848

Reducing Surface Recombination Velocity of Methylammonium-Free Mixed-Cation Mixed-Halide Perovskites via Surface Passivation

Journal Article · Wed Jun 16 00:00:00 EDT 2021 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c00848· OSTI ID:1806288

^[1]; Burke, Sven ^[2]; ^[3]; ^[4]; Taddei, Margherita ^[5]; ^[5]; ^[6]; ^[4]; ^[7]; ^[5]

Univ. of Washington, Seattle, WA (United States); University of Washington
Univ. of Washington, Seattle, WA (United States); Carnegie Mellon Univ., Pittsburgh, PA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Univ. of Arizona, Tucson, AZ (United States)
Univ. of Washington, Seattle, WA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Swift Solar Inc., San Carlos, CA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

We control surface recombination in the mixed-cation, mixed-halide perovskite, FA_0.83Cs_0.17Pb(I_0.85Br_0.15)₃, by passivating nonradiative defects with the polymerizable Lewis base (3-aminopropyl)trimethoxysilane (APTMS). We demonstrate average minority carrier lifetimes >4 μs, nearly single exponential monomolecular photoluminescence decays, and high external photoluminescence quantum efficiencies (>20%, corresponding to ~97% of the maximum theoretical quasi-Fermi-level splitting) at low excitation fluence. We confirm both the composition and valence band edge position of the FA_0.83Cs_0.17Pb(I_0.85Br_0.15)₃ perovskite using multi-institutional, cross-validated, X-ray photoelectron spectroscopy and UV photoelectron spectroscopy measurements. We extend the APTMS surface passivation to higher bandgap double-cation (FA and Cs) compositions (1.7, 1.75, and 1.8 eV) as well as the widely used triple-cation (FA, MA, and Cs) composition. Finally, we demonstrate that the average surface recombination velocity decreases from ~1000 to ~10 cm/s post APTMS passivation for FA_0.83Cs_0.17Pb(I_0.85Br_0.15)₃. Our results demonstrate that surface-mediated recombination is the primary nonradiative loss pathway in many methylammonium (MA)-free mixed-cation mixed-halide films with a range of different bandgaps, which is a problem observed for a wide range of perovskite active layers and reactive electrical contacts. Furthermore, our study also provides insights to develop passivating molecules that help reduce surface recombination in MA-free mixed-cation mixed-halide films and indicates that surface passivation and contact engineering will enable near-theoretical device efficiencies with these materials.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; National Science Foundation

Grant/Contract Number:: EE0008747; AC36-08GO28308

OSTI ID:: 1806288

Alternate ID(s):: OSTI ID: 1812704
OSTI ID: 1910155

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 13 Vol. 33; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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