Abstract
The production of the state of spin alignment of molecules in the lowest triplet state at low temperatures is discussed. The conditions under which microwave, radiation of resonance frequencies with the zerofield (zf) transitions of these molecules would result in an observed change in the phosphorescence intensity are specified. The basic equations relating these intensity changes to unimolecular rate constants are derived. The application of phosphorescence-microwave double resonance (PMDR) spectroscopy to determine the different properties of the triplet state is summarized. A new and convenient magnetic axis system for discussing the zf levels of π, π* triplet states is introduced. The more recent applications of PMDR in determining triplet state geometry as well as the mechanisms of inter- and intramolecular energy transfer processes are discussed in detail.
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