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Ultrafast Enhancement of Ferromagnetic Spin Exchange Induced by Ligand-to-Metal Charge Transfer

Ron, A. and Chaudhary, S. and Zhang, G. and Ning, H. and Zoghlin, E. and Wilson, S. D. and Averitt, R. D. and Refael, G. and Hsieh, D. (2020) Ultrafast Enhancement of Ferromagnetic Spin Exchange Induced by Ligand-to-Metal Charge Transfer. Physical Review Letters, 125 (19). Art. No. 197203. ISSN 0031-9007. doi:10.1103/PhysRevLett.125.197203.

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We theoretically predict and experimentally demonstrate a nonthermal pathway to optically enhance superexchange interaction energies in a material based on exciting ligand-to-metal charge-transfer transitions, which introduces lower-order virtual hopping contributions that are absent in the ground state. We demonstrate this effect in the layered ferromagnetic insulator CrSiTe₃ by exciting Te-to-Cr charge-transfer transitions using ultrashort laser pulses and detecting coherent phonon oscillations that are impulsively generated by superexchange enhancement via magneto-elastic coupling. This mechanism kicks in below the temperature scale where short-range in-plane spin correlations begin to develop and disappears when the excitation energy is tuned away from the charge-transfer resonance, consistent with our predictions.

Item Type:Article
Related URLs:
URLURL TypeDescription Paper
Ron, A.0000-0002-1840-7824
Zoghlin, E.0000-0002-8160-584X
Averitt, R. D.0000-0003-0451-1935
Hsieh, D.0000-0002-0812-955X
Additional Information:© 2020 American Physical Society. Received 10 December 2019; revised 17 August 2020; accepted 2 October 2020; published 4 November 2020. This work was supported by ARO MURI Grant No. W911NF-16-1-0361. D. H. and G. R. also acknowledge support from the David and Lucile Packard Foundation. D. H. acknowledges support for instrumentation from the Institute for Quantum Information and Matter, an NSF Physics Frontiers Center (PHY-1733907). A. R. acknowledges support from the Caltech Prize Fellowship, the Zuckerman Foundation, and the Israel Science Foundation (Grant No. 1017/20). The MRL Shared Experimental Facilities are supported by the MRSEC Program of the NSF under Grant No. DMR 1720256, a member of the NSF-funded Materials Research Facilities Network. S. D. W. acknowledges support from the Nanostructures Cleanroom Facility at the California NanoSystems Institute (CNSI). G. R. also acknowledges partial support through DOE Award No. DE-SC0019166.
Group:Institute for Quantum Information and Matter
Funding AgencyGrant Number
Army Research Office (ARO)W911NF-16-1-0361
David and Lucile Packard FoundationUNSPECIFIED
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
Zuckerman FoundationUNSPECIFIED
Israel Science Foundation1017/20
California NanoSystems InstituteUNSPECIFIED
Department of Energy (DOE)DE-SC0019166
Issue or Number:19
Record Number:CaltechAUTHORS:20191217-085020547
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100322
Deposited By: Tony Diaz
Deposited On:17 Dec 2019 18:06
Last Modified:16 Nov 2021 17:53

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