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

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.