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Title: Temperature-Dependent Optical and Structural Properties of Chiral Two-Dimensional Hybrid Lead-Iodide Perovskites

Journal Article · · Journal of Physical Chemistry. C

Layered hybrid halide perovskites gain chirality via the incorporation of chiral organic cations in the spacer layer. These so-called chiral two-dimensional (2D) halide perovskites have attracted considerable interest recently for chiral optoelectronic, spintronic, and ferroelectric applications. However, the effect of temperature on these materials, especially how the structure changes with temperature and its impact on the chiral optoelectronic properties, remains an open question. Here, we study the effect of temperature change on chiral optoelectronic and structural properties through temperature-dependent circularly polarized photoluminescence (CPPL) microscopy and synchrotron powder X-ray diffraction as well as pair distribution function analysis to elucidate the intrinsic chiral optoelectronic and structural variations for R-, S-, and racemic-methylbenzylamine lead iodide. Here our results show that the temperature-induced band gap changes indicate a strong electron–phonon coupling compared to the thermal-induced lattice expansion in chiral 2D perovskites. From powder diffraction measurements, a monotonic lattice expansion is observed on heating with no structural phase transitions over 90–360 K detected for the three samples studied herein. Locally, a strongly anisotropic and even negative expansion in some components of the instantaneous Pb–I pair-distance distribution is suggestive of coupling between dynamical intralayer distortions and lattice expansion. This work provides insights into the fundamental understanding of the temperature effect on chiral optoelectronic and structural properties of chiral 2D perovskites, which can lead to new chiral materials design strategies for future chiral optoelectronic applications.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)
Grant/Contract Number:
SC0012704
OSTI ID:
1995476
Report Number(s):
BNL-224673-2023-JAAM
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 31 Vol. 127; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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