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Dual Resonant Sum Frequency Generations from Two-Dimensional Materials
- Dual Resonant Sum Frequency Generations from Two-Dimensional Materials
- Kim, Youngjae; Kim, Hyunmin; Jang, Houk; Ahn, Jong-Hyun; Lee, JaeDong
- DGIST Authors
- Kim, Hyunmin; Lee, JaeDong
- Issue Date
- Nano Letters, 20(6), 4530-4536
- Article Type
- Author Keywords
- SFG; dual resonance; excitonic resonance; TMD; rt-TDDFT
- STIMULATED-EMISSION; MOS2
- We propose dual resonant optical sum frequency generation (SFG), where the two most singular resonances could be selected, and report for the monolayer (1L-) WSe2 when one (ω1) of two excitation pulses is resonant to A exciton and their sum frequency (ω1 + ω2) to D exciton. The dual resonant SFG confirms that, under an irradiation of ω1 and ω2 pulses with the same fluence of ∼1.4 × 1010 W/m2, its signal intensity could be enhanced about 20 times higher than the resonant SHG (i.e., 2ω1 to the D excitonic absorption). Further, the dual resonant SFG intensity of 1L-WSe2 is found to be 1 order of magnitude higher than the single resonant SFG intensity of 1L-WS2 under the same condition of two-pulse irradiation. Finally, observations of the dual resonant SFG are thoroughly examined using real-time time-dependent density functional theory (rt-TDDFT), and the relevant nonlinear optical characteristics are scrutinized using the Greenwood-Kubo formalism. Copyright © 2020 American Chemical Society.
- American Chemical Society
- Related Researcher
Light and Matter Theory Laboratory
Theoretical Condensed Matter Physics; Ultrafast Dynamics and Optics; Nonequilibrium Phenomena
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