Orbital-Dependent Photodynamics of Strongly Correlated Clusters
2021
Understanding the role of defect sites on the mechanism and lifetime of photoexcited state relaxation is critical for the ration-al design of advanced materials. Here, the ultrafast electronic relaxation dynamics of neutral nickel oxide clusters were inves-tigated with femtosecond pump-probe spectroscopy and supported with theoretical calculations to reveal that their excited state lifetimes are strongly dependent on the nature of the electronic transition. Absorption of a UV photon produces short lived (lifetime ~110 fs) dynamics in stoichiometric (NiO)n clusters (n 2.5 ps) states. The atomic precision and tunability of gas phase clusters are employed to highlight a unique reliance on the Ni orbital contributions to the photoexcited lifetimes, providing new insights to the anal-ogous band edge excitation dynamics of strongly correlated bulk-scale NiO materials.
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