Semiclassical description of electron spin motion in radicals including the effect of electron hopping

Klaus Schulten, Peter G. Wolynes

The Journal of Chemical Physics · 1978 · 392 citations · 6 references

Concepts

TL;DR

Electron spin dynamics in radicals are driven by hyperfine coupling to nuclear spins and are modeled semiclassically. The authors model electron spin precession around fixed classical nuclear spin vectors, average over configurations to obtain the spin correlation tensor, and incorporate electron hopping via a rotational‑diffusion framework to study singlet‑state radical pair dynamics.

Abstract

The coherent electron spin motion in radicals induced by the hyperfine coupling to nuclear spins is described semiclassically. The nuclear spins are treated as constant classical vectors around which the electron spin precesses. The ensemble average over all nuclear spin configurations is taken yielding the electron spin correlation tensor <S(0)S(t) ≳. Borrowing from the theory of rotational diffusion the effect of electron hopping between molecules on the spin correlation tensor is described. The treatment is applied to the time evolution of the electron spin state of a radical pair initially prepared in a singlet state.

References

6