Highly Distorted Chiral Two-Dimensional Tin Iodide Perovskites for Spin Polarized Charge Transport

Haipeng Lu, Chuanxiao Xiao, Ruyi Song, Tianyang Li, Annalise Maughan, Andrew Levin, Roman Brunecky, Joseph Berry, David Mitzi, Volker Blum, Matthew Beard

Research output: Contribution to journalArticlepeer-review

208 Scopus Citations

Abstract

Incorporating chiral organic molecules into organic/inorganic hybrid 2D metal-halide perovskites results in a novel family of chiral hybrid semiconductors with unique spin-dependent properties. The embedded chiral organic moieties induce a chiroptical response from the inorganic metal-halide sublattice. However, the structural interplay between the chiral organic molecules and the inorganic sublattice, as well as their synergic effect on the resulting electronic band structure need to be explored in a broader material scope. Here we present three new layered tin iodide perovskites templated by chiral (R/S-)methylbenzylammonium (R/S-MBA), i.e., (R-/S-MBA)2SnI4, and their racemic phase (rac-MBA)2SnI4. These MBA2SnI4 compounds exhibit the largest level of octahedral bond distortion compared to any other reported layered tin iodide perovskite. The incorporation of chiral MBA cations leads to circularly polarized absorption from the inorganic Sn-I sublattice, displaying chiroptical activity in the 300-500 nm wavelength range. The bandgap and chiroptical activity are modulated by alloying Sn with Pb, in the series of (MBA)2Pb1-xSnxI4. Finally, we show that vertical charge transport through oriented (R-/S-MBA)2SnI4 thin films is highly spin-dependent, arising from a chiral-induced spin selectivity (CISS) effect. We demonstrate a spin-polarization in the current-voltage characteristics as high as 94%. Our work shows the tremendous potential of these chiral hybrid semiconductors for controlling both spin and charge degrees of freedom.

Original languageAmerican English
Pages (from-to)13030-13040
Number of pages11
JournalJournal of the American Chemical Society
Volume142
Issue number30
DOIs
StatePublished - 29 Jul 2020

Bibliographical note

Publisher Copyright:
Copyright © 2020 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-76598

Keywords

  • chiral
  • emergent optoelectronic applications
  • perovskites
  • transport spin-polarization

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