Abstract
A trimer of dicyanoaurate has been studied as a model system of the covalent chemical bond formation. Here, we report the dynamics of dicyanoaurate trimer in water upon photoexcitation by femtosecond time-resolved luminescence (TL) and luminescence spectra at cyrogenic temperature. Temperature was varied as a means to control the medium flexibility as well as the population of isomers. A unique parallelism between the luminescence spectrum vs. time and vs. temperaturewas observed, which enables unambiguous luminescence band assignments and facilitates investigation of the dynamics. Upon photoexcitation to S1, intersystem crossing proceeds in an ultrafast manner within 20 fs due to the large spin-orbit coupling followed by a structural change from a loose bent to a tight linear form in 1.5 ps. Higher oligomerization occurs above the melting temperature. TL reveals a strong coherent excitation of the symmetric Au-Au stretching vibration at 74 cm-1 through the non-Condon effect.
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