A comparison of generalized cumulant and projection operator methods in spin-relaxation theory

Abstract

The general spin‐relaxation theories of Albers and Deutch and of Argyres and Kelley based on different projection operator methods, and the theory of Freed based on generalized cumulant expansions are compared. It is shown that the first two yield equivalent expressions for the time evolution of the spin density matrix. They are also found to be equivalent to a cumulant expansion based on total ordering of the cumulant operators (TTOC), which is different from the partial time ordering method (PTOC) used by Freed. The TTOC method is found to be the more convenient for the frequency domain (i.e., for calculating spectra), while the PTOC method is for time domain analyses. Examples of the use of the TTOC method are given. Useful expressions are given for the case where the lattice may be treated in terms of classical Markov processes, but, in general, it is found that for such cases the stochastic Liouville method is the more useful for computations.