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Keldysh Space Control of Charge Dynamics in a Strongly Driven Mott Insulator

Li, Xinwei and Ning, Honglie and Mehio, Omar and Zhao, Hengdi and Lee, Min-Cheol and Kim, Kyungwan and Nakamura, Fumihiko and Maeno, Yoshiteru and Cao, Gang and Hsieh, David (2022) Keldysh Space Control of Charge Dynamics in a Strongly Driven Mott Insulator. Physical Review Letters, 128 (18). Art. No. 187402. ISSN 0031-9007. doi:10.1103/physrevlett.128.187402.

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The fate of a Mott insulator under strong low frequency optical driving conditions is a fundamental problem in quantum many-body dynamics. Using ultrafast broadband optical spectroscopy, we measured the transient electronic structure and charge dynamics of an off-resonantly pumped Mott insulator Ca₂RuO₄. We observe coherent bandwidth renormalization and nonlinear doublon-holon pair production occurring in rapid succession within a sub-100-fs pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh crossover from a multiphoton absorption to quantum tunneling dominated pair production regime. Our results provide a procedure to control coherent and nonlinear heating processes in Mott insulators, facilitating the discovery of novel out-of-equilibrium phenomena in strongly correlated systems.

Item Type:Article
Related URLs:
URLURL TypeDescription Paper
Li, Xinwei0000-0003-0555-2624
Zhao, Hengdi0000-0003-4606-6323
Lee, Min-Cheol0000-0002-9145-9700
Kim, Kyungwan0000-0003-3833-5378
Maeno, Yoshiteru0000-0002-3467-9416
Cao, Gang0000-0001-9779-430X
Hsieh, David0000-0002-0812-955X
Additional Information:© 2022 American Physical Society. (Received 24 October 2021; revised 20 February 2022; accepted 11 April 2022; published 6 May 2022) We thank Swati Chaudhary, Nicolas Tancogne-Dejean, and Tae Won Noh for useful discussions. The first-principles calculations in this work were performed using the quantum espresso package. Time-resolved spectroscopic measurements were supported by the Institute for Quantum Information and Matter (IQIM), a NSF Physics Frontiers Center (PHY-1733907). D. H. also acknowledges support for instrumentation from the David and Lucile Packard Foundation and from ARO MURI Grant No. W911NF-16-1-0361. X. L. acknowledges support from the Caltech Postdoctoral Prize Fellowship and the IQIM. G. C. acknowledges NSF support via Grant No. DMR 1903888. M.-C. L. acknowledges funding supports from the Research Center Program of IBS (Institute for Basic Science) in Korea (IBS-R009-D1). K. K. was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2020R1A2C3013454). Y. M. was supported by the JSPS Core-to-Core Program No. JPJSCCA20170002 as well as the JSPS Kakenhi No. JP17H06136.
Group:Institute for Quantum Information and Matter
Funding AgencyGrant Number
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
David and Lucile Packard FoundationUNSPECIFIED
Army Research Office (ARO)W911NF-16-1-0361
Caltech Postdoctoral FellowshipUNSPECIFIED
Institute for Basic Science (Korea)IBS-R009-D1
National Research Foundation of Korea2020R1A2C3013454
Japan Society for the Promotion of Science (JSPS)JPJSCCA20170002
Japan Society for the Promotion of Science (JSPS)JP17H06136
Issue or Number:18
Record Number:CaltechAUTHORS:20220525-286273000
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114906
Deposited By: George Porter
Deposited On:31 May 2022 20:12
Last Modified:31 May 2022 20:12

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