Atomically phase-matched second-harmonic generation in a 2D crystal

Mervin Zhao; Ziliang Ye; Ryuji Suzuki; Yu Ye; Hanyu Zhu; Jun Xiao; Yuan Wang; Yoshihiro Iwasa; Xiang Zhang

doi:10.1038/lsa.2016.131

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Atomically phase-matched second-harmonic generation in a 2D crystal

Original Articles

- Atomically phase-matched second-harmonic generation in a 2D crystal
- Light: Science & Applications Vol. 5, Issue 3, (2016)
- Affiliations：
  
  1.Department of Mechanical Engineering, NSF Nanoscale Science and Engineering Center, University of California, Berkeley, CA 94720, USA
  2.Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA
  3.Quantum-Phase Electronics Center (QPEC) and Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan
  4.RIKEN Center for Emergent Matter Science (CEMS), Wako 351-0198, Japan
  5.Department of Physics, King Abdulaziz University, Jeddah 21589, Saudi Arabia
- Author bio：
  
  X Zhang, Email: xiang@berkeley.edu
- Funds：
- DOI：10.1038/lsa.2016.131
  CLC：
- Published：2016-09，
  
  Published Online：14 March 2016，
  
  Received：21 September 2015，
  
  Revised：07 March 2016，
  
  Accepted：07 March 2016
- Accepted：
Scan QR Code
Zhao, M. et al. Atomically phase-matched second-harmonic generation in a 2D crystal. Light: Science & Applications, 5, e16131 (2016).
DOI：

Zhao, M. et al. Atomically phase-matched second-harmonic generation in a 2D crystal. Light: Science & Applications, 5, e16131 (2016). DOI： 10.1038/lsa.2016.131.

摘要

Abstract

Second-harmonic generation (SHG) has found extensive applications from hand-held laser pointers to spectroscopic and microscopic techniques. Recently

some cleavable van der Waals (vdW) crystals have shown SHG arising from a single

atomic layer

where the SH light elucidated important information such as the grain boundaries and electronic structure in these ultra-thin materials. However

despite the inversion asymmetry of the single layer

the typical crystal stacking restores inversion symmetry for even numbers of layers leading to an oscillatory SH response

drastically reducing the applicability of vdW crystals such as molybdenum disulfide (MoS

). Here

we probe the SHG generated from the noncentrosymmetric 3R crystal phase of MoS

. We experimentally observed quadratic dependence of second-harmonic intensity on layer number as a result of atomically phase-matched nonlinear dipoles in layers of the 3R crystal that constructively interfere. By studying the layer evolution of the A and B excitonic transitions in 3R-MoS

using SHG spectroscopy

we also found distinct electronic structure differences arising from the crystal structure and the dramatic effect of symmetry and layer stacking on the nonlinear properties of these atomic crystals. The constructive nature of the SHG in this 2D crystal provides a platform to reliably develop atomically flat and controllably thin nonlinear media.

关键词

Keywords

atomically thinphase-matchingsecond-harmonic generation3R-MoS2

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