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 (CH3NH3)4Cu2Br6 thin films with a zero-dimensional molecular salt structure featuring "isolated" [Cu2Br6]4- 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 [Cu2Br6]4- anion and the (CH3NH3)4Cu2Br6 crystal suggest a strong impact of the crystal environment on the structure of the anion.
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