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

Evan Lafalce, Eric Amerling, Zhi-Gang Yu, Peter C. Sercel, Luisa Whittaker-Brooks and Z. Valy Vardeny ()
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Evan Lafalce: University of Utah
Eric Amerling: University of Utah
Zhi-Gang Yu: Sivananthan Laboratories
Peter C. Sercel: Center for Hybrid Organic Inorganic Semiconductors for Energy
Luisa Whittaker-Brooks: University of Utah
Z. Valy Vardeny: University of Utah

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-28127-9

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