CaltechAUTHORS
Published May 6, 2022 | Version Accepted Version + Published
Journal Article Open

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

Creators

  • 1. ROR icon California Institute of Technology
  • 2. ROR icon University of Colorado Boulder
  • 3. ROR icon Los Alamos National Laboratory
  • 4. ROR icon Institute for Basic Science
  • 5. ROR icon Chungbuk National University
  • 6. ROR icon Kurume Institute of Technology
  • 7. ROR icon Kyoto University

Abstract

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.

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.

Attached Files

Published - PhysRevLett.128.187402.pdf

Accepted Version - 2205.05172.pdf

Files

2205.05172.pdf

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Additional details

Identifiers

Eprint ID
114906
Resolver ID
CaltechAUTHORS:20220525-286273000

Related works

Describes
10.1103/PhysRevLett.128.187402 (DOI)
https://arxiv.org/abs/2205.05172 (URL)

Funding

Institute for Quantum Information and Matter (IQIM)
NSF
PHY-1733907
David and Lucile Packard Foundation
Army Research Office (ARO)
W911NF-16-1-0361
Caltech Postdoctoral Fellowship
NSF
DMR-1903888
Institute for Basic Science (Korea)
IBS-R009-D1
National Research Foundation of Korea
2020R1A2C3013454
Japan Society for the Promotion of Science (JSPS)
JPJSCCA20170002
Japan Society for the Promotion of Science (JSPS)
JP17H06136

Dates

Created
2022-05-31
Created from EPrint's datestamp field
Updated
2022-05-31
Created from EPrint's last_modified field

Caltech Custom Metadata

Caltech groups
Institute for Quantum Information and Matter