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Floquet engineering of strongly driven excitons in monolayer tungsten disulfide

Nature Physics volume 19, pages 171–176 (2023)Cite this article

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Abstract

Interactions of quantum materials with strong laser fields can induce exotic non-equilibrium electronic states1,2,3,4,5,6. Monolayer transition metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement7, offer exceptional opportunities for the Floquet engineering of excitons, which are quasiparticle electron–hole correlated states8. Strong-field driving has the potential to achieve enhanced control of the electronic band structure and thus the possibility of opening a new realm of exciton light–matter interactions. However, a full characterization of strong-field driven exciton dynamics4,9 has been difficult. Here we use mid-infrared laser pulses below the optical bandgap to excite monolayer tungsten disulfide and demonstrate strong-field light dressing of excitons in excess of a hundred millielectronvolts. Our high-sensitivity transient absorption spectroscopy further reveals the formation of a virtual absorption feature below the 1s-exciton resonance, which we assign to a light-dressed sideband from the dark 2p-exciton state. Quantum-mechanical simulations substantiate the experimental results and enable us to retrieve real-space movies of the exciton dynamics. This study advances our understanding of the exciton dynamics in the strong-field regime, showing the possibility of harnessing ultrafast, strong-field phenomena in device applications of two-dimensional materials.

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Fig. 1: Transient absorption spectra of strongly driven excitons in monolayer WS2.
Fig. 2: Light-dressing mechanisms of strongly driven excitons.
Fig. 3: Optical signatures of the field-driven exciton dynamics.
Fig. 4: Snapshots of the exciton wavepacket.

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Data availability

Source data are provided with this paper. All other data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

Code availability

The codes that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

We thank J. Shi and I. Franco for discussions. This work was primarily supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division through the AMOS program. F.L. was supported by the Terman Fellowship and startup funds from the Department of Chemistry at Stanford University. Y.K. acknowledges support from the Urbanek–Chorodow Fellowship at Stanford University and C.H. acknowledges support from the W. M. Keck Foundation and an Alexander von Humboldt Research Fellowship.

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Author notes

  1. These authors contributed equally: Yuki Kobayashi, Christian Heide.

Authors and Affiliations

  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Yuki Kobayashi, Christian Heide, Fang Liu, David A. Reis, Tony F. Heinz & Shambhu Ghimire

  2. Department of Applied Physics, Stanford University, Stanford, CA, USA

    Yuki Kobayashi, Christian Heide, David A. Reis & Tony F. Heinz

  3. Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA

    Amalya C. Johnson

  4. Department of Chemistry, University of Rochester, Rochester, NY, USA

    Vishal Tiwari

  5. Department of Chemistry, Stanford University, Stanford, CA, USA

    Fang Liu

  6. Department of Photon Science, Stanford University, Stanford, CA, USA

    David A. Reis & Tony F. Heinz

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Contributions

Y.K. and C.H. performed the experiments. A.C.J. and F.L. fabricated the sample. Y.K. performed the simulations and analysed the results. F.L., D.A.R., T.F.H. and S.G. supervised the project. V.T. performed supplementary calculations. All authors contributed to the preparation of the manuscript.

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Correspondence to Yuki Kobayashi or Shambhu Ghimire.

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Supplementary Figs. 1–9 and Discussions.

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Source Data Fig. 1e

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Source Data Fig. 3d

Source data for Fig. 3d.

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Kobayashi, Y., Heide, C., Johnson, A.C. et al. Floquet engineering of strongly driven excitons in monolayer tungsten disulfide. Nat. Phys. 19, 171–176 (2023). https://doi.org/10.1038/s41567-022-01849-9

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