On-Surface Chemistry Induced by Long-Lived Excitons: (NO)2 Dissociation on C60

J Phys Chem Lett. 2020 Jul 16;11(14):5490-5496. doi: 10.1021/acs.jpclett.0c01247. Epub 2020 Jun 26.

Abstract

Solid-state excitonic excitations play an increasingly important role in optoelectronic and light harvesting processes due to their ubiquitous presence in dipolar two-dimensional materials. Here we show that long-lived solid-state excitons induce chemical reactions in adsorbed molecules and thus convert light into chemical energy. For the model system (NO)2 dimer adsorbed on ordered c(4×4) C60 films, time-of-flight measurements following UV laser excitation reveal a slow and a fast dissociative desorption channel, which are assigned to intersystem crossing and internal conversion, respectively, by time-dependent density functional theory calculations.