Journal ArticleDOI
Structural dependence of nonlinear-optical properties of methyl-(2,4-dinitrophenyl)-aminopropanoate crystals
J. L. Oudar,Joseph Zyss +1 more
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In this paper, the structural relationship between microscopic and macroscopic tensors is analyzed to characterize the linear and nonlinear-optical properties of molecular crystals exhibiting a strong donor-acceptor intramolecular interaction.Abstract:
We analyze the structural relationship between microscopic and macroscopic tensors which characterize the linear- and nonlinear-optical properties of molecular crystals exhibiting a strong donor-acceptor intramolecular interaction, with particular reference to methyl-(2,4-dinitrophenyl)-aminopropanoate (MAP). The quasiplanar structure of the active part of these molecules results in a strong and characteristic anisotropy of the optical hyperpolarizabilities, which can be traced up to the macroscopic level when taking into account the crystal symmetry as well as the orientation of the molecules in the unit cell. The experimental data on MAP are thoroughly analyzed on this basis, and it is found that a two-dimensional model of the lowest-order hyperpolarizability tensor results in a structural relation between the macroscopic tensor components, which is in agreement with experimental data. In addition, the principal dielectric axes of this monoclinic crystal are determined by the orientation of the aromatic plane in the unit cell. The overall analysis also enables the determination of four independent components of the molecular hyperpolarizability tensor from experimental data only, and the results have been compared to those of a semiempirical intermediate neglect of differential overlap calculation. The anisotropy of this tensor reveals that the intramolecular charge transfer responsible for the large optical nonlinearity is predominantly from the amino group to the nitro group in para position, rather than towards the nitro group in ortho position. Finally the overall analysis provides a basis for discussing what should be the best orientation of the molecules in the unit cell for maximizing the crystal nonlinearity. The result is that phase-matchable nonlinear coefficients up to six times larger than in MAP could be observed in compounds with similar molecular hyperpolarizabilities but an optimum crystal structure.read more
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Journal ArticleDOI
Organic Polymeric and Non-Polymeric Materials with Large Optical Nonlinearities
TL;DR: In this paper, the electronic origins of nonlinear optical effects in organic π electronic systems are reviewed, with special emphasis being given to second-order nonlinear effects, and the critical relationships of the propagation characteristics of light to observed non-linear optical effect and to solid-state structure are discussed.
Journal ArticleDOI
Nonlinear optical materials.
TL;DR: Property and important materials constants of current commercial materials and of new, promising, inorganic and organic molecular and polymeric materials with potential in second- and third-order nonlinear optical applications are presented.
Journal ArticleDOI
Conjugated oligomers with terminal donor-acceptor substitution.
TL;DR: This Review highlights fundamental synthetic strategies for the preparation of such oligomers with n repeat units and the rules that govern their linear and nonlinear optical properties (absorption, frequency doubling and tripling).
Journal ArticleDOI
Chirality and hydrogen bonding in molecular crystals for phase‐matched second‐harmonic generation: N‐(4‐nitrophenyl)‐(L)‐prolinol (NPP)
TL;DR: In this article, the second-harmonic efficiency of a new organic molecular crystal N(4−nitrophenyl)−(L)−prolinol (NPP) was reported.
Journal ArticleDOI
Model system for optical nonlinearities: Asymmetric quantum wells.
Emmanuel Rosencher,Ph. Bois +1 more
TL;DR: Large absorptions have been observed for the first time in GaAs/AlGaAs multiquantum wells (MQW) by West and Eglash by noting the dipole matrix elements associated to these intersubband transitions (ISBT) have the same order of magnitude as the quantum well width leading to extremely large absorption.
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