Terahertz sum-frequency excitation of coherent optical phonons in the two-dimensional semiconductor WSe2

Author:

Kusaba Satoshi12ORCID,Lin Haw-Wei3ORCID,Tamaki Ryo1,Katayama Ikufumi14ORCID,Takeda Jun14ORCID,Blake Geoffrey A.23ORCID

Affiliation:

1. Department of Physics, Graduate School of Engineering Science, Yokohama National University 1 , Yokohama 240-8501, Japan

2. Division of Geological and Planetary Sciences, California Institute of Technology 2 , Pasadena, California 91125, USA

3. Division of Chemistry and Chemical Engineering, California Institute of Technology 3 , Pasadena, California 91125, USA

4. Semiconductor and Quantum Integrated Electronics Research Center, Institute for Multidisciplinary Sciences, Yokohama National University 4 , Yokohama 240-8501, Japan

Abstract

Driving fundamental excitations via strong light fields is one of the most important issues in solid state physics, which opens up new avenues to control material properties. Two-dimensional materials are fruitful platforms for future semiconductor applications, including opto-electronic and phononic devices, yet the phonon dynamics and nonlinear phonon–phonon coupling remain under-explored. Here, we demonstrate coherent phonon excitation in thin films of the layered two-dimensional semiconductor WSe2 induced by intense and broadband ultrafast terahertz (THz) pulses. We performed THz Kerr effect spectroscopy and observed coherent phonon oscillations assigned to the E2g optical phonon mode. The phonon amplitude displays a quadratic THz field strength dependence, indicating a sum-frequency THz excitation process. Furthermore, pump–probe polarization and crystal orientation relationships, supported by symmetry analysis of the nonlinear susceptibility and Raman tensors, provide helpful insight into nonlinear phonon–phonon interactions and potential coherent control schemes for the manipulation of phonon polarization and material properties in WSe2.

Funder

National Science Foundation

National Aeronautics and Space Administration

Japan Society for the Promotion of Science

Ministry of Education

Publisher

AIP Publishing

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