Ultrafast optical excitation of magnons in 2D antiferromagnets via spin torque exerted by photocurrent of excitons: Signatures in charge pumping and THz emission

Abstract: Recent experiments observing femtosecond laser pulse (fsLP) exciting magnons within two-dimensional (2D) antiferromagnetic (AF) semiconductors -- such as CrSBr, NiPS$_3$, and MnPS$_3$, or their van der Waals heterostructures -- suggest exciton-mediation of such an effect. However, its microscopic details remain obscure as resonant coupling of magnons, living in the sub-meV energy range, to excitons, living in \mbox{$\sim 1$ eV} range, can hardly be operative. Here, we develop a quantum transport theory of this effect, in which time-dependent nonequilibrium Green's function (TDNEF) for electrons driven by classical vector potential of fsLP are coupled to the Landau-Lifshitz-Gilbert (LLG) equation describing classical dynamics of localized magnetic moments (LMMs) within 2D AF semiconductor. Our TDNEGF+LLG theory explains how fsLP, with central frequency above the semiconductor gap, generates a photocurrent that subsequently exerts spin-transfer torque (STT) onto LMMs as a genuine nonequilibrium spintronic effect. The collective motion of LMMs analyzed by windowed Fast Fourier transform (FFT) reveals frequencies of excited magnons, as well as their lifetime governed by nonlocal damping due to the bath of electrons. In addition, the TDNEGF part of our TDNEGF+LLG self-consistent loop computes a time-dependent density matrix whose off-diagonal elements are utilized to describe, at the mean-field level, inter-orbital Coulomb interaction binding electrons and holes into excitons. Our TDNEGF+LLG theory predicts how excited magnons {\em pump} charge current into the attached electrodes, or locally within AF semiconductor responsible for microwave emission. The windowed FFT of the former signal contains imprints of excited magnons, as well as their interaction with excitons, which could be exploited as a novel probe in future experiments.