Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets

Abstract

Magneto-optical excitations in antiferromagnetic d systems can originate from a multiplicity of light-spin and spin-spin interactions, as the light and spin degrees of freedom can be entangled. This is exemplified in van der Waals systems with attendant strong anisotropy between in-plane and out-of-plane directions, such as MnPS3 and NiPS3 films studied here. The rich interplay between the magnetic ordering and sub-bandgap optical transitions poses a challenge to resolve the mechanisms driving spin-entangled optical transitions, as well as the single-particle bandgap itself. Here we employ a high-fidelity ab initio theory to find a realistic estimation of the bandgap by elucidating the atom- and orbital-resolved contributions to the fundamental sub-bands. We further demonstrate that the spin-entangled excitations, observable as photoluminescence and absorption resonances, originate from an on-site spin-flip transition confined to a magnetic atom (Mn or Ni). The evolution of the spin-flip transition

11 pages 4 figures

References in corpus (24)

• Quasiparticle Self-Consistent GW Theory
• Dynamical Mean-Field Theory within the Full-Potential Methods: Electronic structure of Ce-115 materials
• Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
• Charge-spin correlation in van der Waals antiferromagenet NiPS3
• Highly Anisotropic Excitons and Multiple Phonon Bound States in a Van der Waals Antiferromagnetic Insulator
• Spin-Induced Linear Polarization of Excitonic Emission in Antiferromagnetic van der Waals Crystals
• Questaal: a package of electronic structure methods based on the linear muffin-tin orbital technique
• Controlling the anisotropy of a van der Waals antiferromagnet with light
• Optical Stabilization of Fluctuating High Temperature Ferromagnetism in YTiO${}_3$
• Controlling magnetic exchange and anisotropy by non-magnetic ligand substitution in layered MPX3 (M = Ni, Mn; X = S, Se)
• QS$G\hat{W}$: Quasiparticle Self consistent $GW$ with ladder diagrams in $W$
• Self-energies in itinerant magnets: A focus on Fe and Ni
• The magnetic dynamics of NiPS${}_3$
• Terahertz field-induced metastable magnetization near criticality in FePS3
• Magnetically propagating Hund's exciton in van der Waals antiferromagnet NiPS3
• Paramagnetic Electronic Structure of CrSBr: Comparison between Ab Initio GW Theory and Angle-Resolved Photoemission Spectroscopy
• Excitons in Bulk and Layered Chromium Tri-Halides: From Frenkel to the Wannier-Mott Limit
• Electronic Structure of Chromium Trihalides beyond Density Functional Theory
• First principles vs second principles: Role of charge self-consistency in strongly correlated systems
• Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr
• Ultrafast laser-induced spin-lattice dynamics in the van der Waals antiferromagnet CoPS3
• A Theory for Colors of Strongly Correlated Electronic Systems
• Thickness dependence of antiferromagnetic phase transition in Heisenberg-type MnPS3
• Microscopic parameters of the van der Waals CrSBr antiferromagnet from microwave absorption experiments

Cited by in corpus (2)

• Spin-flip optical excitations in van der Waals antiferromagnet CrPS${}_4$
• Magnetic Field-Tunable Repulsive Exciton-Exciton Interaction in the van der Waals Antiferromagnet NiPS${}_3$