Nonlinear optical properties of organic and polymeric materials
29 Sep 1983-
About: The article was published on 1983-09-29 and is currently open access. It has received 762 citations till now.
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TL;DR: In this paper, the authors determined the magnitude of the third-order nonlinear optical susceptibilities of vanadylphthalocyanine (VOPc) films grown on KBr and fused silica substrates, using the third harmonic generation method at a wavelength of 1200 nm.
Abstract: We determined the magnitude of the third‐order nonlinear optical susceptibilities χ(3)(−3ω; ω, ω, ω) of vanadyl‐phthalocyanine (VOPc) films grown on KBr and fused silica substrates, using the third harmonic generation method at a wavelength of 1200 nm. The χ(3) value of the film grown epitaxially on KBr was 2.87×10−10 esu, which was greater by a factor of about 7.7 than that of a polycrystalline film grown on fused silica. The enhancement of χ(3) in the epitaxial phase is associated with the optimized orientation of the two‐dimensional π‐electron system in the condensed phase.
65 citations
TL;DR: In this article, a new molecular engineering strategy is proposed that favors the packing of charge-transfer conjugated molecules to enhance their crystalline quadratic nonlinear efficiency, which is shown to have a powder second-harmonic generation efficiency of the same order as that of N-(4-nitrophenyl)-L-prolinol (NPP), i.e., more than 2 orders of magnitude above that of urea.
Abstract: A new molecular engineering strategy is proposed that favors the packing of charge-transfer conjugated molecules to enhance their crystalline quadratic nonlinear efficiency. A highly polar substituent is grafted to an achiral molecule at a position remote from the donor–acceptor π-electron conjugated system. Dipolar interaction forces will act mainly toward the antiparallel coupling of local dipoles, while the remaining nonlinear portion of the molecule is freed, under other influences, to set up a noncentrosymmetric and possibly optimal structure. Among other 4-nitroanilinelike compounds, N-(4-nitrophenyl)-N-methylaminoacetonitrile (NPAN) exemplifies this new approach and is shown to have a powder second-harmonic generation efficiency of the same order as that of N-(4-nitrophenyl)-L-prolinol (NPP), i.e., more than 2 orders of magnitude above that of urea. The nonlinearity of both molecules (vector part of the β tensor projected along the dipole moment) has been measured by use of electric-field induced second-harmonic (EFISH) generation in solution at 1.06 μm. The nonlinearity of the NPAN molecule is roughly half that of NPP, but the transparency range of NPAN is significantly increased toward the UV compared with that of NPP. Two theoretical models, based, respectively, on a finite-field perturbation of the Hartree–Fock equations and on a sum-over-states expansion of tensor β both at a semiempirical level of approximation, are used to compute the coefficients of the first-order hyperpolarizability of NPP and NPAN. A two-level quantum model is used to account for frequency dispersion, and theoretical crystalline coefficients are obtained from an oriented-gas description of the crystal. Theoretical molecular polarizabilities are in satisfactory agreement with the EFISH experimental results. The experimental crystalline nonlinearity of NPP is also well accounted for by calculations, while the optimized nonlinear coefficient dZYY of crystalline NPAN is predicted to be of the order of 140 × 10−9 esu, coming close to that of NPP.
64 citations
01 Jan 2000
TL;DR: An overview of the current status of second-order nonlinear optical organic materials for their use in photonic applications such as optical frequency converters and electro-optic modulators is presented in this paper.
Abstract: This chapter presents an overview of the current status of second-order nonlinear optical organic materials for their use in photonic applications such as optical frequency converters and electro-optic modulators. Special emphasis is placed on the material aspects and a thorough discussion of presently available substances. The potential of organic materials for third-order nonlinear optical applications has been presented in detail in Chap. 2. Earlier reviews of organic nonlinear optical materials covering different physical and material aspects can be found in [3.1–8].
64 citations
TL;DR: In this paper, a nonlinear optical organic material, (-)2-(α-methylbenzylamino)-5-nitropyridine (MBANP), has been comprehensively investigated with the objective of application to frequency doubling of laser diodes.
Abstract: A nonlinear optical organic material, (-)2-(α-methylbenzylamino)-5-nitropyridine (MBANP), has been comprehensively investigated with the objective of application to frequency doubling of laser diodes. Its molecular hyperpolarizability is as large as that of p-nitroaniline. MBANP crystallizes with a highly asymmetric molecular arrangement. The largest nonlinear optical coefficient, d22, is measured to be 60 pm/V. The corresponding figure of merit for frequency doubling at 1.064 µm is 3.5 times larger than that for d33 of LiNbO3. Cerenkov-radiation-type, phase-matched second-harmonic generation has been demonstrated utilizing the d22 coefficient by making use of an appropriate waveguiding structure.
64 citations
TL;DR: In this paper, the electronic third-order nonlinear optical interaction in a solution cast film of a polydiacetylene has been studied by degenerate four wave mixing and the results demonstrate a subpicosecond response and a very high χ(3) value.
Abstract: The electronic third‐order nonlinear optical interaction in a solution cast film of a polydiacetylene has been studied by degenerate four wave mixing. The results demonstrate a subpicosecond response and a very high χ(3) value. The χ(3) value changes considerably during the thermally induced conformational transition in the film in which the effective π‐electron conjugation is reduced.
62 citations