Journal ArticleDOI
Ab initio analytic polarizability, first and second hyperpolarizabilities of large conjugated organic molecules: Applications to polyenes C4H6 to C22H24
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In this article, the static dipole polarizability and second hyperpolarizability tensors are calculated for polyene systems via ab initio coupled-perturbed Hartree-Fock theory.Abstract:
The static dipole polarizability and second hyperpolarizability tensors are calculated for polyene systems via ab initio coupled‐perturbed Hartree–Fock theory. The effect of basis set augmentation on the calculated properties is explored for C4H6 and example basis sets are used to calculate the polarizability and second hyperpolarizability for the longer polyenes: C6H8, C8H10, C10H12, C12H14, C14H16,C16H18, C18H20, C20H22, C22H24. Results for the finite polyenes are extrapolated to predict the unit‐cell polarizability and second hyperpolarizability of infinite polyacetylene. The working equations which take advantage of the 2n+1 theorem of perturbation theory for calculating up to the second hyperpolarizability are given, and their implementation is briefly discussed. In particular it is shown that the implementation is readily amenable to parallel processing.read more
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Quantum-mechanical condensed matter simulations with CRYSTAL
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Assessment of Conventional Density Functional Schemes for Computing the Dipole Moment and (Hyper)polarizabilities of Push−Pull π-Conjugated Systems†
Benoît Champagne,and Eric A. Perpète,Denis Jacquemin,Stan J. A. van Gisbergen and,Evert Jan Baerends,Chirine Soubra-Ghaoui and,Kathleen A. Robins,Bernard Kirtman +7 more
TL;DR: In this paper, it was shown that the C functional has negligible effect on the calculated dipole moment (μ), α, β, and γ whereas the X-part is responsible for the large property overestimations when the size of the system increases.
Journal ArticleDOI
Assessment of Conventional Density Functional Schemes for Computing the Polarizabilities and Hyperpolarizabilities of Conjugated Oligomers: An Ab Initio Investigation of Polyacetylene Chains
Benoît Champagne,E A Perpète,S. J. A. van Gisbergen,Evert Jan Baerends,J. G. Snijders,C. Soubra-Ghaoui,Kathleen A. Robins,Bernard Kirtman +7 more
TL;DR: In this paper, the authors describe the shortsightedness of the XC potentials which are relatively insensitive to the polarization charge induced by the external electric field at the chain ends, and show that the overestimations are not related to the asymptotic behavior of the potential.
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Organic Materials for Third‐Order Nonlinear Optics
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Frequency dependent nonlinear optical properties of molecules: formulation and implementation in the HONDO program
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TL;DR: In this article, the detailed equations for the time-dependent Hartree-Fock treatment of nonlinear properties for perturbations made up of a static electric field and an oscillating field are summarized.
References
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Journal ArticleDOI
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TL;DR: In this article, an extended basis set of atomic functions expressed as fixed linear combinations of Gaussian functions is presented for hydrogen and the first row atoms carbon to fluorine, where each inner shell is represented by a single basis function taken as a sum of four Gaussians and each valence orbital is split into inner and outer parts described by three and one Gaussian function, respectively.
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Nonlinear optical properties of organic molecules and crystals
Daniel S. Chemla,Joseph Zyss +1 more
Journal ArticleDOI
Basis Set Selection for Molecular Calculations
Ernest R. Davidson,David Feller +1 more
TL;DR: In this article, the authors consider the problem of finding a set of functions which is flexible enough to produce 'good' results over a wide range of molecular geometries and is still small enough to leave the problem computationally tractible and economically within reason.