Photoinduced hot electrons are central to plasmon-driven catalysis. Atomically thin Ti3C2O2, with high carrier density and broad optical absorption, offers a promising platform for plasmon-driven reactions. However, comprehensive investigations of its plasmon resonance, hot-carrier generation, and plasmonic catalytic performance remain limited. In this work, real-time time-dependent density functional theory (rt-TDDFT) was employed to study Ti3C2O2's plasmon excitation and hot-carrier generation from nonradiative plasmon damping. The temporal evolution of the dipole moment reveals plasmon resonance in Ti3C2O2, followed by strong plasmon damping that redistributes the stored energy to generate hot carriers. Ti3C2O2 with low oxygen vacancy concentration (Ov-Ti3C2O2) exhibits plasmonic behavior resembling the pristine surface, and the plasmon-generated hot electrons can markedly reduce the dissociation barrier of CO2 at the oxygen vacancy. These findings provide fundamental insights into the plasmonic properties of Ti3C2O2 and how they drive its catalytic performance in surface reactions, which is valuable for advancing plasmon-driven catalysis.
Zhang et al. (Fri,) studied this question.