AI Article Synopsis
- Hybrid organic-inorganic halogenidocuprates based on copper(I) exhibit diverse structures and high photoluminescence (PL) yields, but the emission mechanism is not fully understood.
- Researchers successfully created thin films of (CHNH)CuBr, which contain isolated [CuBr] ions, and measured a notable excited-state lifetime of 114 μs at room temperature.
- Studies using transient absorption methods and theoretical calculations indicate that a long-lived triplet species forms via intersystem crossing, leading to phosphorescence, with significant effects from the surrounding crystal environment on the [CuBr] anion structure.
Article Abstract
Hybrid organic-inorganic halogenidocuprates based on copper(I) represent materials with rich structural diversity and high photoluminescence (PL) quantum yield, yet the mechanism responsible for their efficient, strongly Stokes-shifted emission is still unclear. Here we report the successful preparation of (CHNH)CuBr thin films with a zero-dimensional molecular salt structure featuring "isolated" [CuBr] ions. Time-resolved broadband PL measurements provide an excited-state lifetime of 114 μs at 298 K. Results from femto- to microsecond UV-vis-NIR transient absorption experiments combined with DFT/TDDFT calculations suggest the formation of a long-lived structurally relaxed triplet species through intersystem crossing (61 ps), which almost exclusively decays by phosphorescence. In addition, time scales for structural relaxation and cooling processes are extracted from a global kinetic analysis of the transient spectra. Calculations for the isolated [CuBr] anion and the (CHNH)CuBr crystal suggest a strong impact of the crystal environment on the structure of the anion.
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| http://dx.doi.org/10.1021/acs.jpclett.1c00446 | DOI Listing |
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