Ultrafast enhancement of ferromagnetic spin exchange induced by ligand-to-metal charge transfer

Abstract

Directly modifying spin exchange energies in a magnetic material with light can enable ultrafast control of its magnetic states. Current approaches rely on tuning charge hopping amplitudes that mediate exchange by optically exciting either virtual or real charge-transfer transitions (CT) between magnetic sites. Here we show that when exchange is mediated by a non-magnetic ligand, it can be substantially enhanced by optically exciting a real CT transition from the ligand to magnetic site, introducing lower order virtual hopping contributions. We demonstrate sub-picosecond enhancement in a superexchange dominated ferromagnet CrSiTe3 through this mechanism using phase-resolved coherent phonon spectroscopy. This technique can also be applied in the paramagnetic phase to disentangle light induced exchange modification from other ultrafast effects that alter the magnetization. This protocol can potentially be broadly applied to engineer thermally inaccessible spin Hamiltonians in superexchange dominated magnets.

arXiv comment13 pages main text, 4 figures, 14 pages supplementary information

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Cited by in corpus (17)

• Coherent Helicity-Dependent Spin-Phonon Oscillations in the Ferromagnetic van der Waals Crystal CrI3
• Cavity magnon-polaritons in cuprate parent compounds
• Fermi's golden rule for heating in strongly driven Floquet systems
• Light-Induced Control of Magnetic Phases in Kitaev Quantum Magnets
• Short-range Crystalline Order-Tuned Conductivity in Cr${}_2$Si${}_2$Te${}_6$ van der Waals Magnetic Crystals
• Time-domain study of coupled collective excitations in quantum materials
• Light controlled THz plasmonic time varying media: momentum gaps, entangled plasmon pairs, and pulse induced time reversal
• Pressure tuning of intrinsic and extrinsic sources to the anomalous Hall effect in CrGeTe${}_3$
• Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl${}_3$
• Time, momentum, and energy resolved pump-probe tunneling spectroscopy of two-dimensional electron systems
• Dynamics of photo-induced ferromagnetism in oxides with orbital degeneracy
• A set-up for Hard X-ray Time-resolved Resonant Inelastic X-ray Scattering at SwissFEL
• Controlling topology through targeted composite symmetry manipulation in magnetic systems
• Probing of magnetic dimensional crossover in CrSiTe${}_3$ through picosecond strain pulses
• X-Ray Scattering from Light-Driven Spin Fluctuations in a Doped Mott Insulator
• Band Splitting and Long-lived Carrier Recombination in Ferromagnetic CrSiTe3 Nanosheets
• Time-dependent exchange creates the time-frustrated state of matter