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High-harmonic generation from an atomically thin semiconductor

Nature Physics volume 13, pages 262–265 (2017)Cite this article

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Abstract

High-harmonic generation (HHG) in bulk solids permits the exploration of materials in a new regime of strong fields and attosecond timescales1,2,3,4,5,6. The generation process has been discussed in the context of strongly driven electron dynamics in single-particle bands7,8,9,10,11,12,13,14. Two-dimensional materials exhibit distinctive electronic properties compared to the bulk that could significantly modify the HHG process15,16, including different symmetries17,18,19, access to individual valleys20,21 and enhanced many-body interactions22,23,24,25. Here we demonstrate non-perturbative HHG from a monolayer MoS2 crystal, with even and odd harmonics extending to the 13th order. The even orders are predominantly polarized perpendicular to the pump and are compatible with the anomalous transverse intraband current arising from the material’s Berry curvature, while the weak parallel component suggests the importance of interband transitions. The odd harmonics exhibit a significant enhancement in efficiency per layer compared to the bulk, which is attributed to correlation effects. The combination of strong many-body Coulomb interactions and widely tunable electronic properties in two-dimensional materials offers a new platform for attosecond physics.

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Figure 1: HHG spectrum from monolayer MoS2.
Figure 2: Dependence of HHG on pump intensity for monolayer MoS2.
Figure 3: Dependence of HHG on crystallographic orientation of monolayer MoS2.
Figure 4: Comparison of the HHG efficiency of an isolated monolayer of MoS2 (red bars) with a monolayer of the bulk crystal (blue bars).

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Acknowledgements

This project was supported primarily by the Air Force Office of Scientific Research under Grant Nos. FA9550-14-1-0108 and FA9550-14-1-0268. Additional support for Y.L. and T.F.H. was provided by the AMOS program, Chemical Sciences, Geosciences, and Biosciences Division, Basic Energy Sciences, U.S. Department of Energy under Contract No. DE-AC02-76-SFO0515 and by the Gordon and Betty Moore Foundation’s EPiQS Initiative through Grant No. GBMF4545. S.G. and Y.S.Y. acknowledge the support from the Office of Science Early Career Research Program. We thank P. H. Bucksbaum for useful discussions.

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Authors and Affiliations

  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

    Hanzhe Liu, Yilei Li, Yong Sing You, Shambhu Ghimire, Tony F. Heinz & David A. Reis

  2. Department of Physics, Stanford University, Stanford, California 94305, USA

    Hanzhe Liu

  3. Department of Applied Physics, Stanford University, Stanford, California 94305, USA

    Yilei Li, Tony F. Heinz & David A. Reis

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  1. Hanzhe Liu
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  2. Yilei Li
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  4. Shambhu Ghimire
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Contributions

H.L. and Y.L. contributed equally to this work, built the experimental set-up, carried out the measurements and analysed the data. D.A.R. and T.F.H. conceived the experiment. H.L., Y.L., Y.S.Y., S.G., T.F.H. and D.A.R. contribute to the interpretation of the data. All authors contributed to the discussions and the preparation of the manuscript.

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Correspondence to David A. Reis.

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The authors declare no competing financial interests.

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Liu, H., Li, Y., You, Y. et al. High-harmonic generation from an atomically thin semiconductor. Nature Phys 13, 262–265 (2017). https://doi.org/10.1038/nphys3946

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