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Giant modulation of optical nonlinearity by Floquet engineering

Shan, Jun-Yi and Ye, M. and Chu, H. and Lee, Sungmin and Park, Je-Geun and Balents, L. and Hsieh, D. (2021) Giant modulation of optical nonlinearity by Floquet engineering. Nature, 600 (7888). pp. 235-239. ISSN 0028-0836. doi:10.1038/s41586-021-04051-8. https://resolver.caltech.edu/CaltechAUTHORS:20211209-456366000

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Abstract

Strong periodic driving with light offers the potential to coherently manipulate the properties of quantum materials on ultrafast timescales. Recently, strategies have emerged to drastically alter electronic and magnetic properties by optically inducing non-trivial band topologies, emergent spin interactions and even superconductivity. However, the prospects and methods of coherently engineering optical properties on demand are far less understood. Here we demonstrate coherent control and giant modulation of optical nonlinearity in a van der Waals layered magnetic insulator, manganese phosphorus trisulfide (MnPS₃). By driving far off-resonance from the lowest on-site manganese d–d transition, we observe a coherent on–off switching of its optical second harmonic generation efficiency on the timescale of 100 femtoseconds with no measurable dissipation. At driving electric fields of the order of 10⁹ volts per metre, the on–off ratio exceeds 10, which is limited only by the sample damage threshold. Floquet theory calculations based on a single-ion model of MnPS₃ are able to reproduce the measured driving field amplitude and polarization dependence of the effect. Our approach can be applied to a broad range of insulating materials and could lead to dynamically designed nonlinear optical elements.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1038/s41586-021-04051-8DOIArticle
https://rdcu.be/cCVvPPublisherFree ReadCube access
https://doi.org/10.1038/s41586-021-04368-4DOIPublisher Correction
https://rdcu.be/cESs9PublisherFree ReadCube access -Publisher Correction
ORCID:
AuthorORCID
Shan, Jun-Yi0000-0001-7665-2169
Chu, H.0000-0002-1989-9517
Park, Je-Geun0000-0002-3930-4226
Balents, L.0000-0002-2377-2711
Hsieh, D.0000-0002-0812-955X
Additional Information:© 2021 Nature Publishing Group. Received 27 April 2021. Accepted 23 September 2021. Published 08 December 2021. Issue Date 09 December 2021. We acknowledge discussions with X. Li, S. Chaudhary and G. Refael. This work was supported by ARO MURI grant number W911NF-16-1-0361. D.H. also acknowledges support for instrumentation from the David and Lucile Packard Foundation and from the Institute for Quantum Information and Matter, an NSF Physics Frontiers Center (PHY-1733907). M.Y. acknowledges support by the Gordon and Betty Moore Foundation through grant GBMF8690 to UCSB and by the National Science Foundation under grant number NSF PHY-1748958. J.-G.P. was supported by the Leading Researcher Program of the National Research Foundation of Korea (grant number 2020R1A3B2079375). Data availability. All other data that support the findings of this study are available from the corresponding author on reasonable request. Source data are provided with this paper. Contributions. S.L. and J.-G.P. synthesized and characterized the MnPS₃ crystals. J.-Y.S. and H.C. performed the optical measurements. M.Y., J.-Y.S. and L.B. performed the single-ion model based static and Floquet dynamical calculations. J.-Y.S., M.Y. and D.H. wrote the paper with input from all authors. Peer review information. Nature thanks thanks Liang Wu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Peer reviewer reports are available. The authors declare no competing interests.
Errata:Shan, JY., Ye, M., Chu, H. et al. Publisher Correction: Giant modulation of optical nonlinearity by Floquet engineering. Nature (2022). https://doi.org/10.1038/s41586-021-04368-4
Group:Institute for Quantum Information and Matter
Funders:
Funding AgencyGrant Number
Army Research Office (ARO)W911NF-16-1-0361
David and Lucile Packard FoundationUNSPECIFIED
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
NSFPHY-1733907
Gordon and Betty Moore FoundationGBMF8690
NSFPHY-1748958
National Research Foundation of Korea2020R1A3B2079375
Issue or Number:7888
DOI:10.1038/s41586-021-04051-8
Record Number:CaltechAUTHORS:20211209-456366000
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20211209-456366000
Official Citation:Shan, JY., Ye, M., Chu, H. et al. Giant modulation of optical nonlinearity by Floquet engineering. Nature 600, 235–239 (2021). https://doi.org/10.1038/s41586-021-04051-8
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112320
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:10 Dec 2021 19:41
Last Modified:01 Feb 2022 22:57

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