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Dynamics of flexible triplet biradicals

Journal Article · · Accounts of Chemical Research; (USA)
DOI:https://doi.org/10.1021/ar00162a001· OSTI ID:7196516

A large number of thermal and photochemical reactions proceed via biradical intermediates. Typically, a biradical generated in the triplet state must first undergo intersystem crossing (ISC) to the singlet biradical before forming products. This presents one of the major challenges of photochemistry; to understand a reaction in which the molecule must hop from one potential energy surface to another. In this Account we are concerned with triplet-derived flexible chain biradicals, and Scheme I shows the important processes. A triplet precursor (e.g., an {sup 3}n, {pi}* ketone) cleaves with conservation of spin to produce a triplet biradical in a set of conformations where the radical centers are close together. Two processes ensue: ISC in a given conformation produces a singlet biradical in the same conformation, and internal rotation gives rise to chain dynamics, which changes the end-to-end distance.

OSTI ID:
7196516
Journal Information:
Accounts of Chemical Research; (USA), Journal Name: Accounts of Chemical Research; (USA) Vol. 22:6; ISSN ACHRE; ISSN 0001-4842
Country of Publication:
United States
Language:
English