Transient Kinetics And Quantum Yield Studies Of Nanocrystalline Alpha-Phenyl-Substituted Ketones: Sorting Out Reactions From Singlet And Triplet Excited States
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY(2018)
摘要
Recent work has shown that diarylmethyl radicals generated by pulsed laser excitation in nanocrystalline (NC) suspensions of tetraarylacetones constitute a valuable probe for the detailed mechanistic analysis of the solid-state photo-decarbonylation reaction. Using a combination of reaction quantum yields and laser flash photolysis in nanocrystalline suspensions of ketones with different substituents on one of the alpha-carbons, we are able to suggest with confidence that a significant fraction of the initial alpha-cleavage reaction takes place from the ketone singlet excited state, that the originally formed diarylmethyl-acyl radical pair loses CO in the crystal with time constants in the sub-nanosecond regime, and that the secondary bis(diarylmethyl) triplet radical pair has a lifetime limited by the rate of intersystem crossing of ca. 70 ns.
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