DOI: https://doi.org/10.29363/nanoge.hpatom.2022.015
Publication date: 30th October 2021
Crystals lacking inversion symmetry have long attracted interest for the properties they can exhibit, from circular dichroism to piezo-, pyro-, and ferro-electricity. Heavy noncentrosymmetric materials displaying Rashba-Dresselhaus effects (momentum-dependent lifting of spin degeneracy via the spin-orbit interaction) are specifically sought as one route to new information processing devices that couple charge and spin. Guided by the chemistry and bonding of Sn(II), we uncover via dielectric and nonlinear optical spectroscopies the previously unstudied polar, chiral ground state phase of perovskite CsSnBr3, which exhibits a bulk Rashba effect. Optical and Mössbauer spectroscopies, X-ray diffraction, and first-principles phonon mode mapping suggest a crystal structure combining octahedral tilting and complex electric dipole order, with unprecedented noncollinear order in two dimensions and ferroic order in the third. 119Sn nuclear magnetic resonance (NMR) spectroscopy and AC transport measurements indicate a complex distribution of free carriers and mobile point defects. We compare the switchabillity of the polarization and spin texture of this phase to the champion bulk Rashba semiconductors and discuss implications for recent claims in other perovskite halides.
D. F. gratefully acknowledges financial support from the Alexander von Humboldt foundation.
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