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

doi:10.34133/2021/9820716

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

Research Article | Updated：2024-10-21

- Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides
- Ultrafast Science Vol. 2021, Issue 2, (2021)
- Affiliations：
  
  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025USA
  2. Department of Applied Physics, Stanford University, Stanford,CA,USA,94305
  3. Max Planck Institute for the Physics of Complex Systems, Nöthnitzer Str. 38, DresdenGermany,01187
  4. Department of Materials Science and Engineering, Stanford University, Stanford,CA,USA,94305
  5. Department of Chemistry, Stanford University, Stanford,CA,USA,94305
  6. Department of Photon Science, Stanford University, Stanford,CA,USA,94305
- Author bio：
- Funds：
- DOI：10.34133/2021/9820716
  CLC：
- Published：2021，
- Accepted：
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YUKI KOBAYASHI, CHRISTIAN HEIDE, HAMED KOOCHAKI KELARDEH, et al. Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides. [J]. Ultrafast science, 2021, 2021(2).
DOI：

YUKI KOBAYASHI, CHRISTIAN HEIDE, HAMED KOOCHAKI KELARDEH, et al. Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides. [J]. Ultrafast science, 2021, 2021(2). DOI： 10.34133/2021/9820716.

摘要

Abstract

We present a systematic study of the crystal-orientation dependence of high-harmonic generation in monolayer transition-metal dichalcogenides

WS and MoSe

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 WS

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 MoSe 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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Keywords

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