Pseudo-Stilbene- and Azobenzene-Type Systems for Optical Frequency Conversion: Estimating the First-Order Molecular Hyperpolarizability

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Artigo
Data de publicação
2024
Periódico
Photonics
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2
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Araujo R.S.
Rodrigues J.J.
Alencar M.A.R.C.
Rafique J.
Saba S.
Abegao L.M.G.
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© 2024 by the authors.This study investigates the potential of a set of pseudo-stilbene and azobenzene molecular structures to become optical frequency converters for optical communications based on a detailed exploration of the first-order molecular hyperpolarizability ((Formula presented.)), which is the microscopic counterpart of second harmonic generation (SHG). (Formula presented.) values were obtained via quantum chemical calculations using the Gaussian 16 software package in solvent and gas-phase media at different wavelengths, i.e., 1064 nm, 1310 nm, and 1510 nm. The latter two wavelengths are of particular interest for optical communications. Our study focused on discerning how the molecular structure influences the (Formula presented.) response, explicitly highlighting the influence of the azomethine group (CH=N). The results revealed that the molecular planarity, affected by this group, plays a crucial role in modulating the optical properties. The highest (Formula presented.) value in a solvent medium using the CAM-B3LYP/6-311+G(2d,p) level of theory achieved in this work was around (Formula presented.), four orders of magnitude higher than KDP (0.2 (Formula presented.)), which is a reference in SHG experiments at 1064 nm. The highest calculated (Formula presented.) value at the same level of theory and solvent at 1310 nm and 1550 nm was (Formula presented.) and (Formula presented.), respectively. All these values belong to molecular structures with azo-coupling with donor (4-NMe2) and acceptor (4′-NO2) peripheral groups, designated as AB-3.
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