Energy Level Gradients from Surface to Bulk in Hybrid Metal-Halide Perovskite Thin Films

Bourelle, Sean A.; Zhang, Xie; Feldmann, Sascha; Zhang, Baiyu; Mathieson, Angus; Eyre, Lissa; Abolins, Haralds; Winkler, Thomas; Van de Walle, Chris G.; Deschler, Felix

doi:10.1103/PRXEnergy.3.033001

Title: Energy Level Gradients from Surface to Bulk in Hybrid Metal-Halide Perovskite Thin Films

Journal Article · 25 July 2024 · PRX Energy

DOI: https://doi.org/10.1103/PRXEnergy.3.033001 · OSTI ID:2474169

Bourelle, Sean A.;

;

; Zhang, Baiyu; Mathieson, Angus; Eyre, Lissa; Abolins, Haralds; Winkler, Thomas;

;

Variations in local strain, defect densities, and composition of hybrid metal-halide perovskites have been reported to create heterogeneous energy landscapes in thin films, which impact charge-carrier diffusion and recombination dynamics. Here, we employ one- and two-photon transient absorption spectroscopy to selectively probe the dynamics of charge carriers from surface and bulk regions of methylammonium lead bromide thin films. Differences in the transient absorption spectra indicate that an energy gradient of approximately 100 meV is formed between the higher band-gap surface and lower band-gap bulk regions. Thus, during their lifetime, photoexcited carriers move away from the surface to recombine in the bulk, where our experiments detect long-lived charge populations despite the significant band splitting that has conventionally been assumed to inhibit efficient radiative recombination. Supported by first-principles calculations, we demonstrate that bright emission can still arise from the bulk with states that occupy a wide range of momenta in the vicinity of the band extrema, which show strong dipole transitions. Our results report that photoexcitations in the hybrid perovskites avoid defect-rich surface regions, and that particularly strong emission is generated from accumulated excitation populations in the bulk. Published by the American Physical Society 2024

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0010689

OSTI ID:: 2474169

Journal Information:: PRX Energy, Journal Name: PRX Energy Journal Issue: 3 Vol. 3; ISSN 2768-5608

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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