Hyperfine-induced spin relaxation of a diffusively moving carrier in low dimensions: implications for spin transport in organic semiconductors

TL;DR

This paper models hyperfine-induced spin relaxation of carriers performing random walks in low-dimensional organic semiconductors, revealing superexponential decay, field sensitivity, and the impact of self-intersections on spin transport.

Contribution

It provides a theoretical analysis of spin relaxation in low dimensions, highlighting the role of random walk returns and external fields in spin dynamics of organic semiconductors.

Findings

Superexponential decay of spin polarization in 1D and 2D systems.

Sensitivity of spin relaxation to external electric and magnetic fields.

Dependence of spin decay length on external fields and dimensionality.

Abstract

The hyperfine coupling between the spin of a charge carrier and the nuclear spin bath is a predominant channel for the carrier spin relaxation in many organic semiconductors. We theoretically investigate the hyperfine-induced spin relaxation of a carrier performing a random walk on a d-dimensional regular lattice, in a transport regime typical for organic semiconductors. We show that in d=1 and d=2 the time dependence of the space-integrated spin polarization, P(t), is dominated by a superexponential decay, crossing over to a stretched exponential tail at long times. The faster decay is attributed to multiple self-intersections (returns) of the random walk trajectories, which occur more often in lower dimensions. We also show, analytically and numerically, that the returns lead to sensitivity of P(t) to external electric and magnetic fields, and this sensitivity strongly depends on dimensionality of the system (d=1 vs. d=3). Furthermore, we investigate in detail the coordinate dependence of the time-integrated spin polarization, $\sigma(r)$, which can be probed in the spin transport experiments with spin-polarized electrodes. We demonstrate that, while $\sigma(r)$ is essentially exponential, the effect of multiple self-intersections can be identified in transport measurements from the strong dependence of the spin decay length on the external magnetic and electric fields.