Abstract

The search for advanced optical materials, in particular, materials with nonlinear optical responses, has, in the last years, experienced substantial growth due to their vast applications in the photonics field. One of those applications is ultra-fast optical frequency conversion, in the optics communications field. Organic compounds have emerged as promising candidates for raw materials to develop nonlinear optical devices, such as optical converters, due to their intrinsic ultra-fast electronic responses. Also, the easy tailoring of organic molecular structures makes organic materials much more appealing than the inorganic ones. In this work, we have performed a linear and nonlinear optical characterization of a set of dibenzylideneacetone derivatives. The nonlinear optical responses investigated correspond to second- and third-order nonlinear processes, namely, first electronic molecular hyperpolarizability and two-photon absorption cross-section, respectively. The value of the first electronic molecular hyperpolarizability, up to 52 cm4·statvolt−1, could be considered a robust value when compared to the short-sized π-electron backbone length of the studied compounds. Such results suggest that these compounds exhibit the potential to be used as optical frequency converters. Quantum chemical calculations were used to predict the theoretical value of the first molecular hyperpolarizability, as well as to simulate the one- and two-photon absorption spectra for all compounds.

Highlights

  • The evolution of optical communication networks demands the search and development of raw materials with particular types of nonlinear optical (NLO) properties with the potential to be used as optical communication devices

  • We report the second- and third-order nonlinear optical properties of the dibenzylideneacetone-substituted compounds in a dichloromethane solution

  • The ε value is neglible for wavelengths longer than 450 nm, making these samples extremely suitable for hyper-Rayleigh scattering (HRS) measurement when pumped with a pulsed laser at 1064 nm

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Summary

Introduction

The evolution of optical communication networks demands the search and development of raw materials with particular types of nonlinear optical (NLO) properties with the potential to be used as optical communication devices. Larger molecules are generally more challenging to combine in a dense solid-state, such as a crystal [9,10,11], representing a drawback to achieving the final photonic product Another approach for improving the performance of the SHG response is to modify the charge density asymmetry of the compound by adding donor and acceptor peripherals groups on its molecular structure [12,13,14]. This latter approach probably will not be as effective in terms of achieving high values of polarizability, as is the case with increasing the π-conjugation length, but will overcome the issue of growth crystal, allowing one to reach a final product with more ease

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