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

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.0c03899· OSTI ID:1660032

Incorporating chiral organic molecules into organic/inorganic hybrid 2D-layered 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.

Research Organization:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1660032
Report Number(s):
NREL/JA-5900-76598; MainId:7272; UUID:105d88b4-dabe-498d-a583-03d054c8fdd5; MainAdminID:13795
Journal Information:
Journal of the American Chemical Society, Vol. 142, Issue 30; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 108 works
Citation information provided by
Web of Science

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