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    Nonlinear Optical Imaging, Precise Layer Thinning, and Phase Engineering in MoTe2 with Femtosecond Laser
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    Abstract:
    The control of layer thickness and phase structure in two-dimensional transition metal dichalcogenides (2D TMDCs) like MoTe2 has recently gained much attention due to their broad applications in nanoelectronics and nanophotonics. Continuous-wave laser-based thermal treatment has been demonstrated to realize layer thinning and phase engineering in MoTe2, but requires long heating time and is largely influenced by the thermal dissipation of the substrate. The ultrafast laser produces a different response but is yet to be explored. In this work, we report the nonlinear optical interactions between MoTe2 crystals and femtosecond (fs) laser, where we have realized the nonlinear optical characterization, precise layer thinning, and phase transition in MoTe2 using a single fs laser platform. By using the fs laser with a low fluence as an excitation light source, we observe the strong nonlinear optical signals of second-harmonic generation and four-wave mixing in MoTe2, which can be used to identify the odd–even layers and layer numbers, respectively. With increasing the laser fluence to the ablation threshold (Fth), we achieve layer-by-layer removal of MoTe2, while 2H-to-1T′ phase transition occurs with a higher laser fluence (2Fth to 3Fth). Moreover, we obtain highly ordered subwavelength nanoripples on both the thick and few-layer MoTe2 with a controlled fluence, which can be attributed to the fs laser-induced reorganization of the molten plasma. Our study provides a simple and efficient ultrafast laser-based approach capable of characterizing the structures and modifying the physical properties of 2D TMDCs.
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    Thinning
    We will present the most recent results on the growth and characterization of novel high quality molecular crystals for nonlinear optics. These crystals are based on ionic or hydrogen bonding of new and known chromophores with large second-order hyperpolarizabilities. Detailed results of optical, electro-optical and nonlinear-optical properties of high quality and large size DAST crystals, of hydrazone derivatives and new co-crystals will be presented. It will be shown that optimized parallel alignment of chromophores as well as optimum structures for phase-matched frequency mixing have been realized. In addition, we report on the measurement of the highest known phase-matchable nonlinear susceptibility coefficient of 200 pm/v determined recently in our laboratory.
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    Optical materials
    In order to design new organic NLO materials with both higher nonlinear optical susceptibilities, and reasonable optical loss characteristics, it is necessary to understand how different organic structural elements affect the nonlinearity of materials at the molecular level. Only recently, synthetic research groups have begun to devote the time and effort necessary to produce very pure model compounds of systematically varied structures for carefully controlled NLO measurements. In this presentation experimental results and the structural- NLO property trends developed from them are reviewed for the systematic investigations appearing in the literature with emphasis placed on studies conducted by our research group. With these results in mind, some new ways of looking at such organic molecular structures are presented with the intent of stimulating creative thought for novel NLO molecular design.
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    Abstract Only NONLINEAROPTICAL PROPERTIES AND NONUNEAR OPTICAL PROBES OF ORGANICMATERIALS Gerald R. MeredithCentral Research and Development Department The DuPont Co.Wilmington, Delaware 19880-0356 Nonlinear optical processes and electro-oplical effects are expected to have increasingimportance as the information age matures and photonics augnnt electronics in various highdensity and high bandwidth technologies. Whereas for electronics the emphasis is in construction of smaller device structures from a few parent materials, for organic materials thedirection of materials research has been reversed. For some time it's been known that somemolecular structures engender exceptionally large molecular nonlinear-polarization responses.If such molecules could be assembled in convenient, versatile and reliable ways, the resultingmaterials would be very useful or even enabling in various photonics applications. The maturescience and art of chemistry allows very good control over molecular composition and structure
    Optical materials
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