Temperature-Dependent Reversible Optical Properties of Mn-Based Organic-Inorganic Hybrid (C8H20N)2MnCl4 Metal Halides

ACS Appl Mater Interfaces. 2023 Feb 1;15(4):5487-5494. doi: 10.1021/acsami.2c20885. Epub 2023 Jan 18.

Abstract

Organic-inorganic metal halides (OIMHs) have abundant optical properties and potential applications, such as light-emitting diodes, displays, solar cells, and photodetectors. Herein, we report zero-dimensional Mn-based OIMH (C8H20N)2MnCl4 single crystals synthesized by a simple slow evaporation method, which exhibit intense green emission at 520 nm originating from 4T1-6A1 transition of Mn2+ ions. Large organic cations in the crystal structure result in the isolated [MnCl4]2- tetrahedrons, and the closest Mn-Mn distance reaches 9.07 Å, which effectively inhibits the migration of excitation energy between adjacent Mn2+ emission centers, thus achieving a high quantum yield (∼87%) and a long photoluminescence (PL) lifetime (3.42 ms). The different optical and structural properties at low and high temperatures are revealed by temperature-dependent PL and X-ray diffraction spectra. The PL spectra and lifetimes under the heating and cooling processes indicate that the optical property transitions are reversible at 220/240 K. Our work provides a promising strategy for building multifunctional optoelectronic materials and insights into the understanding convertible photophysical properties from isomers of metal halides.

Keywords: 0D metal halides; convertible photophysical properties; lead-free; light-emitting diode; manganese halide.