Abstract
Multi-element two-dimensional (2D) materials hold great promise in the context of tailoring the physical and chemical properties of the materials via stoichiometric engineering. However, the rational and controllable synthesis of complex 2D materials remains a challenge. Herein, we demonstrate the preparation of large-area thin quaternary 2D material flakes via mechanical exfoliation from a naturally occurring bulk crystal named gillulyite. Furthermore, the anisotropic linear and nonlinear optical properties including anisotropic Raman scattering, linear dichroism, and anisotropic third-harmonic generation (THG) of the exfoliated gillulyite flakes are investigated. The observed highly anisotropic optical properties originate from the reduced in-plane crystal symmetry. Additionally, the third-order nonlinear susceptibility of gillulyite crystal is retrieved from the measured thickness-dependent THG emission. We anticipate that the demonstrated strong anisotropic linear and nonlinear optical responses of gillulyite crystal will facilitate the better understanding of light-matter interaction in quaternary 2D materials and its implications in technological innovations such as photodetectors, frequency modulators, nonlinear optical signal processors, and solar cell applications.
Highlights
Ranging from energy storage to security purposes such as thermoelectrics, laser frequency modulators, radiation sensors, and photovoltaics[23,24,25]
Here we explore the anisotropic linear and nonlinear optical responses of mechanically exfoliated gillulyite thin flakes
These results will facilitate the fundamental understanding of light-matter interaction in quaternary 2D materials and advance future technological innovations in photonics and optoelectronics such as photodetection, frequency conversion, nonlinear optical signal processing, and photonic circuits
Summary
Ranging from energy storage to security purposes such as thermoelectrics, laser frequency modulators, radiation sensors, and photovoltaics[23,24,25]. The insightful understanding of light-matter interaction associated with the structural properties of these materials will be valuable for their engagement in technological improvisation To address these issues, here we explore the anisotropic linear and nonlinear optical responses of mechanically exfoliated gillulyite thin flakes. We demonstrate that it is relatively easy to mechanically exfoliate the naturally occurring bulk gillulyite crystal into large-area thin flakes with sizes of tens of micrometers down to deep-subwavelength scale thicknesses. To obtain further intuitive understanding, the thirdorder nonlinear susceptibility tensor elements are estimated by corroborating the measured THG signal with a theoretical nonlinear model These results will facilitate the fundamental understanding of light-matter interaction in quaternary 2D materials and advance future technological innovations in photonics and optoelectronics such as photodetection, frequency conversion, nonlinear optical signal processing, and photonic circuits
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