Chirality-Induced Spin Coherence in Electron Transfer Reactions.

Recently, there has been much interest in the chirality-induced spin selectivity effect, whereby electron spin polarization, which is dependent on molecular chirality, is produced in electrode-molecule electron transfer processes. Naturally, one might consider if a similar effect can be observed in simple molecular charge transfer reactions, for example, in light-induced electron transfer from an electron donor to an electron acceptor. In this work, I explore the effect of electron transfer on spins in chiral single radicals and chiral radical pairs using Nakajima-Zwanzig theory. In these cases, chirality, in conjuction with spin-orbit coupling, does not lead to spin polarization, but instead, the electron transfer generates quantum coherence between spins states. In principle, this chirality-induced spin coherence could manifest in a range of experiments, and in particular, I demonstrate that the out of phase electron spin echo envelope modulation pulse electron paramagnetic resonance experiment would be able to detect this effect in oriented radical pairs.