Coherence in multilevel systems

Mathematical descriptions of an excited state multilevel system are developed to include progressively the effects of coherent coupling, feeding, decay and relaxation, and the expressions are illustrated with several pulse coherence experiments utilizing zero field optically detected magnetic resonance of excited triplet states. A new method is described in which the time development of the coherent components in a multilevel system is monitored by using an observable that can measure only relative populations between the levels. The method is illustrated. By treating a coherently driven excited state system as two levels in contact with a population reservoir, exact expressions are obtained for both transient and steady-state behavior in the presence of transverse and spin lattice relaxation, constant incoherent pumping, spontaneous emission between the two levels, and also decay back into the reservoir. The general mathematical development is applied specifically to zero field microwave phosphorescence double resonance. Experimental methods and apparatus are discussed in detail and results of optically detected transient mutations, spin echoes, and Fourier transform spectroscopy are presented. (26 figs, 220 refs) (auth