Spin Dynamics in Radical Pairs by Alan Lewis

Author:Alan Lewis
Language: eng
Format: epub, pdf
ISBN: 9783030006860
Publisher: Springer International Publishing

While the positions and heights of the resonance peaks in the triplet yields of both wires are captured well by these calculations, there is very poor agreement between experiment and theory in the high field region. We believe that this discrepancy suggests that the reaction scheme in Fig. 4.1 is incomplete; specifically, it is missing a magnetic field independent “background” contribution to the yield of D–B–A. In the absence of such a background, one would expect the high field triplet yield to be approximately one third of its zero-field value. This is a result of the high field effect described in Sect. 1.​3.​1: two of the three triplet states have a much larger energy gap to the singlet state in the high field limit than when there is no applied field, so intersystem crossing to those states will be significantly reduced. This argument is consistent with the raw simulations of the relative triplet yields in Fig. 4.4, which are tending towards a value of around in the high field limit. However, it is clearly inconsistent with experimentally measured relative triplet yields.

The discrepancies between our simulations and the experiments are resolved if we assume that the experiments are detecting an additional contribution to the triplet yield produced by some field independent process outside of the mechanism outlined in Fig. 4.1. This would in effect add a background contribution to the triplet yields calculated using the radical pair model. To account for this contribution, we have recalculated the relative triplet yield (RTY) as

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