Rashba splitting in organic–inorganic lead–halide perovskites revealed through two-photon absorption spectroscopy

Lafalce, Evan; Amerling, Eric; Yu, Zhi-Gang; Sercel, Peter C.; Whittaker-Brooks, Luisa; Vardeny, Z. Valy

doi:10.1038/s41467-022-28127-9

Title: Rashba splitting in organic–inorganic lead–halide perovskites revealed through two-photon absorption spectroscopy

Journal Article · 24 January 2022 · Nature Communications

DOI: https://doi.org/10.1038/s41467-022-28127-9 · OSTI ID:1842242

; Amerling, Eric;

;

; Whittaker-Brooks, Luisa;

Abstract The Rashba splitting in hybrid organic–inorganic lead–halide perovskites (HOIP) is particularly promising and yet controversial, due to questions surrounding the presence or absence of inversion symmetry. Here we utilize two-photon absorption spectroscopy to study inversion symmetry breaking in different phases of these materials. This is an all-optical technique to observe and quantify the Rashba effect as it probes the bulk of the materials. In particular, we measure two-photon excitation spectra of the photoluminescence in 2D, 3D, and anionic mixed HOIP crystals, and show that an additional band above, but close to the optical gap is the signature of new two-photon transition channels that originate from the Rashba splitting. The inversion symmetry breaking is believed to arise from ionic impurities that induce local electric fields. The observation of the Rashba splitting in the bulk of HOIP has significant implications for the understanding of their spintronic and optoelectronic device properties.

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Research Organization:: University of Utah, Salt Lake City, UT (United States)

Sponsoring Organization:: US Army Research Office (ARO); USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0014579; SC0019041

OSTI ID:: 1842242

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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