Atomically thin transition metal dichalcogenides (TMDs) in their excited states can serve as exceptionally small building blocks for active optical platforms. In this scheme, optical excitation provides a practical approach to control light‐TMD interactions via the photocarrier generation, in an ultrafast manner. Here, it is demonstrated that via a controlled generation of photocarriers the second‐harmonic generation (SHG) from a monolayer MoS2crystal can be substantially modulated up to ≈55% within a timeframe of ≈250 fs, a set of performance characteristics that showcases the promise of low‐dimensional materials for all‐optical nonlinear data processing. The combined experimental and theoretical study suggests that the large SHG modulation stems from the correlation between the second‐order dielectric susceptibility χ(2)and the density of photoexcited carriers in MoS2. Indeed, the depopulation of the conduction band electrons, at the vicinity of the high‐symmetry
A preliminary measurement of the second‐order nonlinear optical susceptibility of symmetric, coupled, InAs/AlSb multiple quantum well (MQW) structures is acquired through optical second‐harmonic generation (SHG) at fundamental wavelength 1.55 µm. High quality crystalline MQW structures of variable thickness and corresponding bulk AlSb control samples are achieved using a digital alloy epitaxial growth technique that avoids cluster formation and phase segregation. All samples are grown in between a GaSb cap and substrate layer. To isolate SHG from the MQW (or control) layers of interest from cap and substrate contributions, a multilayer optical response matrix model is built and independently tested by accurately reproducing linear reflectivity spectra. While a simplified response matrix analysis of SHG based solely on bulk χ(2)s does not reproduce the distinct SHG responses of the two sets of samples, the inclusion of an additional interface SHG contribution leads to a successful fit of the data and implies . The results demonstrate a proof‐of‐concept quantification of χ(2)in symmetric MQWs and suggest the possibility of engineering χ(2)in these structures, particularly with the introduction of well asymmetries.
more » « less- Award ID(s):
- 1838435
- PAR ID:
- 10369539
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Optical Materials
- Volume:
- 10
- Issue:
- 15
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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