Inorganic Chain Mediated Excitonic Properties in One-Dimensional Lead Halide Hybrid Perovskites

Chen Xue; Hengming Huang; Sadafumi Nishihara; Vasudevanpillai Biju; Xiao-Ming Ren; Takayoshi Nakamura

doi:10.1021/acs.jpclett.2c01978

Inorganic Chain Mediated Excitonic Properties in One-Dimensional Lead Halide Hybrid Perovskites

J Phys Chem Lett. 2022 Aug 18;13(32):7405-7412. doi: 10.1021/acs.jpclett.2c01978. Epub 2022 Aug 4.

Authors

Chen Xue^{1

2

3}, Hengming Huang⁴, Sadafumi Nishihara^{5

6}, Vasudevanpillai Biju^{1

2}, Xiao-Ming Ren³, Takayoshi Nakamura^{1

2}

Affiliations

¹ Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0020, Japan.
² Graduate School of Environmental Science, Hokkaido University, Sapporo 060-0810, Japan.
³ State Key Laboratory of Materials-Oriented Chemical Engineering and College of Chemistry and Molecular Engineering, Nanjing Tech University, Nanjing 211816, P. R. China.
⁴ College of Materials Science and Engineering, Nanjing Tech University, Nanjing 211816, P. R. China.
⁵ Department of Chemistry and Center for Chiral Science, Hiroshima University, Higashi-Hiroshima 739-8527, Japan.
⁶ JST, PRESTO, Honcho 4-1-8, Kawaguchi, Saitama 332-0012, Japan.

PMID: 35927064
DOI: 10.1021/acs.jpclett.2c01978

Abstract

Semiconductors that emit intrinsic white light are considered next-generation lighting sources. Herein, the broadband emission of one-dimensional (1D) lead halide perovskites, TMAPbBr_3-xI_x (x = 0, 1, 1.5, 2, 3; TMA⁺ = tetramethylammonium), is systematically investigated. Lattice distortion causes the conversion of dark excitons to bright self-trapped excitons. Owing to its strongly localized exciton recombination and high absorption probability, TMAPbBr₃ is the most viable in this family. A delocalized hole increases the nonradiative recombination rate of excitons in TMAPbBr_3-xI_x alloys. In 1D TMAPbBr_3-xI_x perovskites, the vibration mode of the Pb-X bond stretching of the PbX₆ octahedra contributes more to the effect on exciton-phonon coupling than the mode of the X-Pb-X angle bending. Pb-X bond stretching and spontaneous polarization can tune exciton binding energy. This systematic study of excitonic behavior in 1D compounds relates the nature of ground states to the unknown excited states and provides the rational design of materials with stable and efficient broadband emission.