Mixed Organic Cation in Chiral Two-Dimensional Organic-Inorganic Hybrid Metal Halides: An ab-initio Study of Nonlinear Optical (NLO) Properties

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Main Authors: Cheng, Xiyue, Muthukrishnan, S., Mi, Hanxiang, Deng, Shuiquan, Serdaroglu, Goncagul, Vidya, R., Stroppa, Alessandro
Format: Preprint
Published: 2026
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author Cheng, Xiyue
Muthukrishnan, S.
Mi, Hanxiang
Deng, Shuiquan
Serdaroglu, Goncagul
Vidya, R.
Stroppa, Alessandro
author_facet Cheng, Xiyue
Muthukrishnan, S.
Mi, Hanxiang
Deng, Shuiquan
Serdaroglu, Goncagul
Vidya, R.
Stroppa, Alessandro
contents The mixing of organic cations represents yet another direction to explore in the field of chiral organic-inorganic hybrid metal halides (OIHMH). Here, we perform structural optimizations, electronic structures, and non-linear optical (NLO) studies using the density functional theory of two recently synthesized chiral OIHMHs, [R-MePEA][C3A]PbBr4, and [R-MePEA][C4A]PbBr4, with mixed chiral arylammonium and achiral alkylammonium cations. We find that the noncovalent weak interactions (e.g. Br...NH interactions) play an important role in the formation of these OIHMHs. Our study further indicates that the two non-centrosymmetric compounds exhibit relative wide bandgaps (~3.5 eV), strong second harmonic generation (SHG) responses (~0.5-1.5*KDP), and moderate birefringence (~0.088), indicating possible applications NLO materials. Atom response theory analysis reveals that the SHG responses are determined mainly by the occupied Br 3p non-bonding orbitals as well as by the unoccupied Pb 5p orbitals which shows the important contribution of the inorganic PbBr4 layer to the nonlinear optical properties.
format Preprint
id arxiv_https___arxiv_org_abs_2603_00398
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Mixed Organic Cation in Chiral Two-Dimensional Organic-Inorganic Hybrid Metal Halides: An ab-initio Study of Nonlinear Optical (NLO) Properties
Cheng, Xiyue
Muthukrishnan, S.
Mi, Hanxiang
Deng, Shuiquan
Serdaroglu, Goncagul
Vidya, R.
Stroppa, Alessandro
Materials Science
The mixing of organic cations represents yet another direction to explore in the field of chiral organic-inorganic hybrid metal halides (OIHMH). Here, we perform structural optimizations, electronic structures, and non-linear optical (NLO) studies using the density functional theory of two recently synthesized chiral OIHMHs, [R-MePEA][C3A]PbBr4, and [R-MePEA][C4A]PbBr4, with mixed chiral arylammonium and achiral alkylammonium cations. We find that the noncovalent weak interactions (e.g. Br...NH interactions) play an important role in the formation of these OIHMHs. Our study further indicates that the two non-centrosymmetric compounds exhibit relative wide bandgaps (~3.5 eV), strong second harmonic generation (SHG) responses (~0.5-1.5*KDP), and moderate birefringence (~0.088), indicating possible applications NLO materials. Atom response theory analysis reveals that the SHG responses are determined mainly by the occupied Br 3p non-bonding orbitals as well as by the unoccupied Pb 5p orbitals which shows the important contribution of the inorganic PbBr4 layer to the nonlinear optical properties.
title Mixed Organic Cation in Chiral Two-Dimensional Organic-Inorganic Hybrid Metal Halides: An ab-initio Study of Nonlinear Optical (NLO) Properties
topic Materials Science
url https://arxiv.org/abs/2603.00398