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An optical cycling center (OCC) is a recently coined term to indicate twoelectronic states within a complex quantum object that can repeatedlyexperience optical laser excitation and spontaneous decay, while being wellisolated from its environment. Here we present a quantitative understanding ofelectronic, vibrational, and rotational excitations of the polyatomic SrOHmolecule, which possesses a localized OCC near its Sr atom. In particular, wedescribe the vibrationally-dependent trends in the Franck-Condon factors of thebending and stretching modes of the molecular electronic states coupled in theoptical transition. These simulations required us to perform electronicstructure calculations of the multi-dimensional potential energy surfaces ofboth ground and excited states, the determination of vibrational and bendingmodes, and corresponding Franck-Condon factors. We also discuss the extent towhich the optical cycling center has diagonal Franck-Condon factors.

Emulating optical cycling centers in polyatomic molecules