Spin-Phonon coupling parameters from maximally localized Wannier functions and first principles electronic structure: the case of durene single crystal

TL;DR

This paper develops a method to calculate spin-phonon coupling in organic crystals using first-principles electronic structure and maximally localized Wannier functions, focusing on durene, revealing that internal molecular vibrations dominate the interaction.

Contribution

The paper introduces a novel approach combining density functional theory and Wannier functions to quantify spin-phonon coupling in organic semiconductors.

Findings

Spin-orbit interaction is weak in durene due to small atomic masses.

The dominant spin-phonon coupling arises from internal molecular vibrations.

The method effectively analyzes symmetry and extracts coupling parameters for organic crystals.

Abstract

Spin-orbit interaction is an important vehicle for spin relaxation. At finite temperature lattice vibrations modulate the spin-orbit interaction and thus generate a mechanism for spin-phonon coupling, which needs to be incorporated in any quantitative analysis of spin transport. Starting from a density functional theory \textit{ab initio} electronic structure, we calculate spin-phonon matrix elements over the basis of maximally localized Wannier functions. Such coupling terms form an effective Hamiltonian to be used to extract thermodynamic quantities, within a multiscale approach particularly suitable for organic crystals. The symmetry of the various matrix elements are analyzed by using the $\Gamma$-point phonon modes of a one-dimensional chain of Pb atoms. Then the method is employed to extract the spin-phonon coupling of solid durene, a high-mobility crystal organic semiconducting. Owing to the small masses of carbon and hydrogen spin-orbit is weak in durene and so is the spin-phonon coupling. Most importantly we demonstrate that the largest contribution to the spin-phonon interaction originates from Holstein-like phonons, namely from internal molecular vibrations.