Magnetically propagating Hund's exciton in van der Waals antiferromagnet NiPS3

Abstract

Magnetic van der Waals (vdW) materials have opened new frontiers for realizing novel many-body phenomena. Recently NiPS3 has received intense interest since it hosts an excitonic quasiparticle whose properties appear to be intimately linked to the magnetic state of the lattice. Despite extensive studies, the electronic character, mobility, and magnetic interactions of the exciton remain unresolved. Here we address these issues by measuring NiPS3 with ultra-high energy resolution resonant inelastic x-ray scattering (RIXS). We find that Hund's exchange interactions are primarily responsible for the energy of formation of the exciton. Measuring the dispersion of the Hund's exciton reveals that it propagates in a way that is analogous to a double-magnon. We trace this unique behavior to fundamental similarities between the NiPS3 exciton hopping and spin exchange processes, underlining the unique magnetic characteristics of this novel quasiparticle.

11 pages accepted in Nature Communications

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• Characteristic exciton energy scales in antiferromagnetic NiPS${}_3$
• Long-lived population inversion in resonantly driven excitonic antiferromagnet
• Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl${}_3$
• Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets
• Revealing the Electronic Structure of van der Waals Antiferromagnetic NiPS${}_3$ through Synchrotron-Based $\mu$-ARPES and Alkali Metal Dosing
• Observation of anisotropic dispersive dark exciton dynamics in CrSBr
• Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition
• Crystal field tuned spin-flip luminescence in NiPS3
• Hamiltonian parameter inference from resonant inelastic x-ray scattering with active learning
• Ultrafast Dynamics of Spin-Orbit Entangled Excitons Coupled to Magnetic Ordering in van der Waals Antiferromagnet NiPS3
• Magnetic Field-Tunable Repulsive Exciton-Exciton Interaction in the van der Waals Antiferromagnet NiPS${}_3$