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Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides

Yuki Kobayashi Christian Heide Hamed Koochaki Kelardeh Amalya Johnson Fang Liu Tony F. Heinz David A. Reis Shambhu Ghimire

Yuki Kobayashi, Christian Heide, Hamed Koochaki Kelardeh, Amalya Johnson, Fang Liu, Tony F. Heinz, David A. Reis, Shambhu Ghimire. 2021: Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides. 超快科学, 2021(2). doi: 10.34133/2021/9820716
引用本文: Yuki Kobayashi, Christian Heide, Hamed Koochaki Kelardeh, Amalya Johnson, Fang Liu, Tony F. Heinz, David A. Reis, Shambhu Ghimire. 2021: Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides. 超快科学, 2021(2). doi: 10.34133/2021/9820716
Yuki Kobayashi, Christian Heide, Hamed Koochaki Kelardeh, Amalya Johnson, Fang Liu, Tony F. Heinz, David A. Reis, Shambhu Ghimire. 2021: Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides. Ultrafast Science, 2021(2). doi: 10.34133/2021/9820716
Citation: Yuki Kobayashi, Christian Heide, Hamed Koochaki Kelardeh, Amalya Johnson, Fang Liu, Tony F. Heinz, David A. Reis, Shambhu Ghimire. 2021: Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides. Ultrafast Science, 2021(2). doi: 10.34133/2021/9820716

Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides

doi: 10.34133/2021/9820716
基金项目: 

This work was 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 a Terman Fellowship and startup funds from the Department of Chemistry at Stanford University. Y.K. acknowledges support from the Urbanek-Chodorow Fellowship from Stanford University. C.H. acknowledges support from the W. M. Keck Foundation and a Humboldt Research Fellowship. We thank Dr. S. Azar Oliaei Motlagh for the fruitful discussion on the simulations.

详细信息
    通讯作者:

    Correspondence should be addressed to Shambhu Ghimire

Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides

Funds: 

This work was 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 a Terman Fellowship and startup funds from the Department of Chemistry at Stanford University. Y.K. acknowledges support from the Urbanek-Chodorow Fellowship from Stanford University. C.H. acknowledges support from the W. M. Keck Foundation and a Humboldt Research Fellowship. We thank Dr. S. Azar Oliaei Motlagh for the fruitful discussion on the simulations.

  • 摘要:

    We present a systematic study of the crystal-orientation dependence of high-harmonic generation in monolayer transition-metal dichalcogenides, WS2 and MoSe2, subjected to intense linearly polarized midinfrared laser fields. The measured spectra consist of both odd- and even-order harmonics, with a high-energy cutoff extending beyond the 15th order for a laser-field strength around ~1 V/nm. In WS2, we find that the polarization direction of the odd-order harmonics smoothly follows that of the laser field irrespective of the crystal orientation, whereas the direction of the even-order harmonics is fixed by the crystal mirror planes. Furthermore, the polarization of the even-order harmonics shows a flip in the course of crystal rotation when the laser field lies between two of the crystal mirror planes. By numerically solving the semiconductor Bloch equations for a gapped-graphene model, we qualitatively reproduce these experimental features and find the polarization flipping to be associated with a significant contribution from interband polarization. In contrast, high-harmonic signals from MoSe2 exhibit deviations from the laser-field following of odd-order harmonics and crystal-mirror-plane following of even-order harmonics. We attribute these differences to the competing roles of the intraband and interband contributions, including the deflection of the electron-hole trajectories by nonparabolic crystal bands.

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出版历程
  • 收稿日期:  2021-04-08
  • 修回日期:  2021-06-25
  • 刊出日期:  2021-08-25

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