Influence of Annealing and Composition on the Crystal Structure of Mixed-Halide, Ruddlesden–Popper Perovskites

Wright, Niara E.; Qin, Xixi; Xu, Junwei; Kelly, Leah L.; Harvey, Steven P.; Toney, Michael F.; Blum, Volker; Stiff-Roberts, Adrienne D.

doi:10.1021/acs.chemmater.1c04213

Influence of Annealing and Composition on the Crystal Structure of Mixed-Halide, Ruddlesden–Popper Perovskites

Journal Article · Wed Mar 16 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.1c04213· OSTI ID:1865118

^[1]; Qin, Xixi ^[1]; Xu, Junwei ^[2]; Kelly, Leah L. ^[2]; ^[3]; ^[4]; ^[1]; Stiff-Roberts, Adrienne D. ^[1]

Duke Univ., Durham, NC (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Univ. of Colorado, Boulder, CO (United States)

Mixed-halide two-dimensional (2D) hybrid organic–inorganic perovskites offer an important opportunity to control the band gap for applications in optoelectronic devices. In this study, we focus on phenethylammonium lead halide [(PEA)₂Pb(I_1–xBr_x)₄] films, the pure iodide form of which is one of the most widely studied optically active 2D perovskite systems. Resonant infrared, matrix-assisted pulsed laser evaporation is used to grow films to explore the effects of post-growth annealing and mixed-halide composition. The composition, crystal structure, and optical properties are studied for as-grown and annealed films of (PEA)₂Pb(I_1–xBr_x)₄ for x = 0, 0.25, 0.5, 0.75, and 1. First-principles calculations are used in conjunction with the experimental data to explain the mixed-halide behavior that does not trend monotonically with the bromide content. Important results of this work are as follows: (i) X-ray diffraction reveals evidence for halide phase separation around x = 0.25, consistent with first-principles calculations, whereas no phase separation is observed for x = 0.5 and above and (ii) a unique photoluminescence (PL) peak splitting is observed for x = 0.75, a composition for which no compositional phase separation is observed. The PL splitting is tentatively explained by the coexistence of two distinct types of halide short-range ordering at x = 0.75. Overall, this study demonstrates that mixed-halide n = 1 Ruddlesden–Popper perovskites are not simple random alloys but that instead, they display distinct sites and ordering preferences of the different halide anions. These preferences are critical to understand and rationally tune the properties of the materials.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

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

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; AC36-08GO28308

OSTI ID:: 1865118

Report Number(s):: NREL/JA-5K00-81937; MainId:82710; UUID:c465a4d1-b518-4fd0-9f42-0a5001b6aa13; MainAdminID:64367

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 7 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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