Controlling magnetism with light in a zero orbital angular momentum antiferromagnet

Abstract

Antiferromagnetic materials feature intrinsic ultrafast spin dynamics, making them ideal candidates for future magnonic devices operating at THz frequencies. A major focus of current research is the investigation of optical methods for the efficient generation of coherent magnons in antiferromagnetic insulators. In magnetic lattices endowed with orbital angular momentum, spin-orbit coupling enables spin dynamics through the resonant excitation of low-energy electric dipoles such as phonons and orbital resonances which interact with spins. However, in magnetic systems with zero orbital angular momentum, microscopic pathways for the resonant and low-energy optical excitation of coherent spin dynamics are lacking. Here, we consider experimentally the relative merits of electronic and vibrational excitations for the optical control of zero orbital angular momentum magnets, focusing on a limit case: the antiferromagnet manganese thiophoshate (MnPS3), constituted by orbital singlet Mn2+ ions. We study the correlation of spins with two types of excitations within its band gap: a bound electron orbital excitation from the singlet orbital ground state of Mn2+ into an orbital triplet state, which causes coherent spin precession, and a vibrational excitation of the crystal field that causes thermal spin disorder. Our findings cast orbital transitions as key targets for magnetic control in insulators constituted by magnetic centers of zero orbital angular momentum.

arXiv comment9 pages, 4 figures

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• Direct imaging of antiferromagnetic domains and anomalous layer-dependent mirror symmetry breaking in atomically thin MnPS${}_3$
• Vibrational coherent control of localized d-d electronic excitation

Cited by in corpus (11)

• Ultrafast laser-induced spin-lattice dynamics in the van der Waals antiferromagnet CoPS3
• Orbital Rashba effect as a platform for robust orbital photocurrents
• Exciton-magnon splitting in van der Waals antiferromagnet MnPS${}_3$ unveiled by second-harmonic generation
• Laser-induced Demagnetization in van der Waals $XY$- and Ising-like Antiferromagnets NiPS${}_3$ and FePS${}_3$
• Effect of biquadratic magnetic exchange interaction in the 2D antiferromagnets MPS_3 (M = Mn, Fe, Co, Ni)
• Brightened Optical Transition as Indicator of Multiferroicity in a Layered Antiferromagnet
• Field-induced spin polarization in lightly Cr-substituted layered antiferromagnet NiPS3
• Phonon-driven multipolar dynamics in a spin-orbit coupled Mott insulator
• Optical Spin Sensing and Metamagnetic Phase Control in the 2D Van der Waals Magnet Yb3+-Doped CrPS4
• Spin-flip optical excitations in van der Waals antiferromagnet CrPS${}_4$
• Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet