Thermodynamic Band Gap Model for Photoinduced Phase Segregation in Mixed-Halide Perovskites

Ruth, Anthony; Okrepka, Halyna; Kamat, Prashant; Kuno, Masaru

doi:10.1021/acs.jpcc.3c04708

Thermodynamic Band Gap Model for Photoinduced Phase Segregation in Mixed-Halide Perovskites

Journal Article · Fri Sep 08 00:00:00 EDT 2023 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.3c04708· OSTI ID:2338289

Ruth, Anthony ^[1]; ^[2]; ^[2]; ^[2]

University of Notre Dame, IN (United States); University of Notre Dame
University of Notre Dame, IN (United States)

Provided is a comprehensive description of a band gap thermodynamic model, which predicts and explains key features of photosegregation in lead-based, mixed-halide perovskites. The model gives a prescription for illustrating halide migration driven by photocarrier energies. Where possible, model predictions are compared with experimental results. Free energy derivations are provided for three assumptions: (1) halide mixing in the dark, (2) a fixed number of photogenerated carriers funneling to and localizing in low band gap inclusions of the alloy, and (3) the statistical occupancy of said inclusions from a bath of thermalized photocarriers in the parent material. Model predictions include excitation intensity (I_exc)-dependent terminal halide stoichiometries (x_terminal), temperature-independent x_terminal, excitation intensity thresholds (I_{exc,threshold}) below which photosegregation is suppressed, and reduced segregation in nanocrystals as compared to thin films. Here, the model also offers insight into kinetically manipulating photosegregation rates via control of underlying mediators and rationalizes asymmetries in forward and reverse photosegregation rate constants/activation energies. What emerges is a cohesive framework for understanding ubiquitous photosegregation in mixed-halide perovskites and a rational basis by which to manage the phenomenon.

View Accepted Manuscript (DOE)

Research Organization:: University of Notre Dame, IN (United States)

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

Grant/Contract Number:: SC0014334

OSTI ID:: 2338289

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 37 Vol. 127; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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