Transient X-ray Diffraction Reveals Nonequilibrium Phase Transition in Thin Films of CH3NH3PbI3 Perovskite

Panuganti, Shobhana; Cuthriell, Shelby A.; Leonard, Ariel A.; Quintero, Michael A.; Laing, Craig C.; Guzelturk, Burak; Zhang, Xiaoyi; Chen, Lin X.; Kanatzidis, Mercouri G.; Schaller, Richard D.

doi:10.1021/acsenergylett.2c02338

Transient X-ray Diffraction Reveals Nonequilibrium Phase Transition in Thin Films of CH₃NH₃PbI₃ Perovskite

Journal Article · Thu Dec 22 00:00:00 EST 2022 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.2c02338· OSTI ID:2348918

^[1]; Cuthriell, Shelby A. ^[1]; Leonard, Ariel A. ^[1]; ^[1]; ^[1]; ^[2]; ^[2]; ^[3]; ^[3]; ^[3]

Northwestern Univ., Evanston, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Advantageous optoelectronic properties of methylammonium lead triiodide likely arise from coupling between photogenerated charge-carriers and the soft, deformable lattice. We investigate structural dynamics of MAPbI₃ films using time-resolved X-ray diffraction versus pump-probe time delay and pump intensity. During the first nanosecond, the lattice anisotropically distorts from tetragonal to cubic at excitation intensities that are insufficient to thermally induce the first-order thermodynamic phase transition at 330K. Further, the high-symmetry structure then relaxes back to the starting phase with 11 and 236-ns time constants via a different transition pathway than observed either in the first nanosecond or in previous reports for MAPbI₃. Early-time dynamics are consistent with polaron formation and lattice strain stabilization while the slower recovery dynamics outlive radiative recombination and relates metastability. Fluence-independence of these lattice deformations in the low-power regime conveys relevance to optoelectronics including photovoltaics and highlights sustained involvement of non-equilibrium, photoinduced lattice reorganization in MAPbI₃ under functional conditions.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012541

OSTI ID:: 2348918

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 1 Vol. 8; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Transient X-ray Diffraction Reveals Nonequilibrium Phase Transition in Thin Films of CH3NH3PbI3 Perovskite

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Transient X-ray Diffraction Reveals Nonequilibrium Phase Transition in Thin Films of CH₃NH₃PbI₃ Perovskite