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Title: Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling

Abstract

Abstract Translation of chirality and asymmetry across structural motifs and length scales plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. Here, we introduce a structural chirality transfer across the organic–inorganic interface in two-dimensional hybrid perovskites using appropriate chiral organic cations. The preferred molecular configuration of the chiral spacer cations, R -(+)- or S -(−)-1-(1-naphthyl)ethylammonium and their asymmetric hydrogen-bonding interactions with lead bromide-based layers cause symmetry-breaking helical distortions in the inorganic layers, otherwise absent when employing a racemic mixture of organic spacers. First-principles modeling predicts a substantial bulk Rashba-Dresselhaus spin-splitting in the inorganic-derived conduction band with opposite spin textures between R - and S -hybrids due to the broken inversion symmetry and strong spin-orbit coupling. The ability to break symmetry using chirality transfer from one structural unit to another provides a synthetic design paradigm for emergent properties, including Rashba-Dresselhaus spin-polarization for hybrid perovskite spintronics and related applications.

Authors:
ORCiD logo; ; ORCiD logo; ; ORCiD logo; ; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1664450
Alternate Identifier(s):
OSTI ID: 1816369
Grant/Contract Number:  
AC36-08G028308; AC02-05CH11231; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 11 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Jana, Manoj K., Song, Ruyi, Liu, Haoliang, Khanal, Dipak Raj, Janke, Svenja M., Zhao, Rundong, Liu, Chi, Valy Vardeny, Z., Blum, Volker, and Mitzi, David B. Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling. United Kingdom: N. p., 2020. Web. doi:10.1038/s41467-020-18485-7.
Jana, Manoj K., Song, Ruyi, Liu, Haoliang, Khanal, Dipak Raj, Janke, Svenja M., Zhao, Rundong, Liu, Chi, Valy Vardeny, Z., Blum, Volker, & Mitzi, David B. Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling. United Kingdom. https://doi.org/10.1038/s41467-020-18485-7
Jana, Manoj K., Song, Ruyi, Liu, Haoliang, Khanal, Dipak Raj, Janke, Svenja M., Zhao, Rundong, Liu, Chi, Valy Vardeny, Z., Blum, Volker, and Mitzi, David B. Thu . "Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling". United Kingdom. https://doi.org/10.1038/s41467-020-18485-7.
@article{osti_1664450,
title = {Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling},
author = {Jana, Manoj K. and Song, Ruyi and Liu, Haoliang and Khanal, Dipak Raj and Janke, Svenja M. and Zhao, Rundong and Liu, Chi and Valy Vardeny, Z. and Blum, Volker and Mitzi, David B.},
abstractNote = {Abstract Translation of chirality and asymmetry across structural motifs and length scales plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. Here, we introduce a structural chirality transfer across the organic–inorganic interface in two-dimensional hybrid perovskites using appropriate chiral organic cations. The preferred molecular configuration of the chiral spacer cations, R -(+)- or S -(−)-1-(1-naphthyl)ethylammonium and their asymmetric hydrogen-bonding interactions with lead bromide-based layers cause symmetry-breaking helical distortions in the inorganic layers, otherwise absent when employing a racemic mixture of organic spacers. First-principles modeling predicts a substantial bulk Rashba-Dresselhaus spin-splitting in the inorganic-derived conduction band with opposite spin textures between R - and S -hybrids due to the broken inversion symmetry and strong spin-orbit coupling. The ability to break symmetry using chirality transfer from one structural unit to another provides a synthetic design paradigm for emergent properties, including Rashba-Dresselhaus spin-polarization for hybrid perovskite spintronics and related applications.},
doi = {10.1038/s41467-020-18485-7},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United Kingdom},
year = {2020},
month = {9}
}

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