Abstract
An improved analysis is presented for the kinetic traces of the electron spin resonance (ESR) signal intensity of photoexcited triplet states during and after a rectangular light pulse. It is assumed that the mixing ratio ξp, defined by 〈1‖1〉=ξp(q‖q)+(1−ξp)(r‖r) and 〈−1‖−1〉=(1−ξp)(q‖q)+ξp(r‖r), deviates from 1/2, where ‖1〉, ‖0〉, ‖−1〉, and ‖p), ‖q), ‖r) are the spin wave functions for the triplet sublevels with and without an external magnetic field parallel to the p principal molecular axis with p, q, r=x,y,z or a cyclic permutation thereof. An X-band ESR experiment is done for the chlorophyll-a (Chla) triplet state in a methanol–methylene chloride glassy matrix at 77 K. Previous theory fits the y and z components but not the x component. This failure can be attributed to the fact that ξp≠1/2, and the improved analysis fits well for the x component as well as the y and z components with ξx=0.555±0.010.
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