Self-Trapped, Thermally Equilibrated Delayed Fluorescence Enables Low-Reabsorption Luminescent Solar Concentrators Based on Gold-Doped Silver Nanoclusters

Abstract

Reabsorption-free luminescent solar concentrators (LSCs) are crucial ingredients for photovoltaic windows. Atomically precise metal nanoclusters (NCs) with large Stokes-shifted photoluminescence (PL) hold great promise for applications in LSCs. However, a fundamental understanding of the PL mechanism, particularly on the excited-state interaction and exciton kinetics, is still lacking. Herein, we studied the exciton-phonon coupling and singlet/triplet exciton dynamics for gold-doped silver NCs in a solid matrix. Following photoexcitation, the excitons can be self-trapped via strong exciton-phonon coupling. Subsequently, rapid thermal equilibration between the singlet and triplet states occurs due to the coexistence of small energy splitting and spin-orbit coupling. Finally, broadband delayed fluorescence with a large Stokes shift can be generated, namely, self-trapped, thermally equilibrated delayed fluorescence (ST-TEDF). Benefiting from superior ST-TEDF, we demonstrated efficient LSCs with minimized reabsorption.

Keywords: Stokes shift; luminescent solar concentrators; metal nanoclusters; self-trapped excitons; thermally equilibrated delayed fluorescence.