Continuous Wave Sum Frequency Generation and Imaging of Monolayer and Heterobilayer Two-Dimensional Semiconductors

Yao, Kaiyuan; Yanev, Emanuil; Chuang, Hsun-Jen; Rosenberger, Matthew R.; Xu, Xinyi; Darlington, Thomas; McCreary, Kathleen M.; Hanbicki, Aubrey T.; Watanabe, Kenji; Taniguchi, Takashi; Jonker, Berend T.; Zhu, Xiaoyang; Basov, D. N.; Hone, James C.; Schuck, P. James

doi:10.1021/acsnano.9b07555

Title: Continuous Wave Sum Frequency Generation and Imaging of Monolayer and Heterobilayer Two-Dimensional Semiconductors

Journal Article · 30 December 2019 · ACS Nano

DOI: https://doi.org/10.1021/acsnano.9b07555 · OSTI ID:1767655

Yao, Kaiyuan ^[1]; Yanev, Emanuil ^[2]; Chuang, Hsun-Jen ^[3];

^[3]; Xu, Xinyi ^[2]; Darlington, Thomas ^[4];

^[3]; Hanbicki, Aubrey T. ^[5]; Watanabe, Kenji ^[6]; Taniguchi, Takashi ^[6]; Jonker, Berend T. ^[3];

^[2]; Basov, D. N. ^[2]; Hone, James C. ^[2];

^[2]

Columbia Univ., New York, NY (United States); Univ. of California, Berkeley, CA (United States); OSTI
Columbia Univ., New York, NY (United States)
Naval Research Lab. (NRL), Washington, DC (United States)
Columbia Univ., New York, NY (United States); Univ. of California, Berkeley, CA (United States)
Naval Research Lab. (NRL), Washington, DC (United States); Univ. of Maryland, College Park, MD (United States)
National Inst. for Materials Science (NIMS), Tsukuba (Japan)

Here, we report continuous-wave second harmonic and sum frequency generation from two-dimensional transition metal dichalcogenide monolayers and their heterostructures with pump irradiances several orders of magnitude lower than those of conventional pulsed experiments. The high nonlinear efficiency originates from above-gap excitons in the band nesting regions, as revealed by wavelength-dependent second order optical susceptibilities quantified in four common monolayer transition metal dichalcogenides. Using sum frequency excitation spectroscopy and imaging, we identify and distinguish one- and two-photon resonances in both monolayers and heterobilayers. Data for heterostructures reveal responses from constituent layers accompanied by nonlinear signal correlated with interlayer transitions. We demonstrate spatial mapping of heterogeneous interlayer coupling by sum frequency and second harmonic confocal microscopy on heterobilayer MoSe₂/WSe₂.

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Research Organization:: Columbia Univ., New York, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Programmable Quantum Materials (Pro-QM)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019443

OSTI ID:: 1767655

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 1 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Continuous Wave Sum Frequency Generation and Imaging of Monolayer and Heterobilayer Two-Dimensional Semiconductors

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