Highly Distorted Chiral Two-Dimensional Tin Iodide Perovskites for Spin Polarized Charge Transport
Abstract
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 semiconductorsmore »
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Duke Univ., Durham, NC (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1660032
- Report Number(s):
- NREL/JA-5900-76598
Journal ID: ISSN 0002-7863; MainId:7272;UUID:105d88b4-dabe-498d-a583-03d054c8fdd5;MainAdminID:13795
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 30; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chiral; emergent optoelectronic applications; perovskites; transport spin-polarization
Citation Formats
Lu, Haipeng, Xiao, Chuanxiao, Song, Ruyi, Li, Tianyang, Maughan, Annalise E., Levin, Andrew, Brunecky, Roman, Berry, Joseph J., Mitzi, David B., Blum, Volker, and Beard, Matthew C. Highly Distorted Chiral Two-Dimensional Tin Iodide Perovskites for Spin Polarized Charge Transport. United States: N. p., 2020.
Web. doi:10.1021/jacs.0c03899.
Lu, Haipeng, Xiao, Chuanxiao, Song, Ruyi, Li, Tianyang, Maughan, Annalise E., Levin, Andrew, Brunecky, Roman, Berry, Joseph J., Mitzi, David B., Blum, Volker, & Beard, Matthew C. Highly Distorted Chiral Two-Dimensional Tin Iodide Perovskites for Spin Polarized Charge Transport. United States. https://doi.org/10.1021/jacs.0c03899
Lu, Haipeng, Xiao, Chuanxiao, Song, Ruyi, Li, Tianyang, Maughan, Annalise E., Levin, Andrew, Brunecky, Roman, Berry, Joseph J., Mitzi, David B., Blum, Volker, and Beard, Matthew C. Tue .
"Highly Distorted Chiral Two-Dimensional Tin Iodide Perovskites for Spin Polarized Charge Transport". United States. https://doi.org/10.1021/jacs.0c03899. https://www.osti.gov/servlets/purl/1660032.
@article{osti_1660032,
title = {Highly Distorted Chiral Two-Dimensional Tin Iodide Perovskites for Spin Polarized Charge Transport},
author = {Lu, Haipeng and Xiao, Chuanxiao and Song, Ruyi and Li, Tianyang and Maughan, Annalise E. and Levin, Andrew and Brunecky, Roman and Berry, Joseph J. and Mitzi, David B. and Blum, Volker and Beard, Matthew C.},
abstractNote = {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.},
doi = {10.1021/jacs.0c03899},
journal = {Journal of the American Chemical Society},
number = 30,
volume = 142,
place = {United States},
year = {Tue Jun 30 00:00:00 EDT 2020},
month = {Tue Jun 30 00:00:00 EDT 2020}
}
Web of Science
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