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Quadratic and Cubic Nonlinearities in Solution of Intramolecular Charge Transfer Aromatic Molecules A Quantum Two-Level Approach

Published online by Cambridge University Press:  25 February 2011

M. Barzoukas ,
P. Fremaux ,
D. Josse ,
F. Kajzar  and
J. Zyss
M. Barzoukas
Affiliation:
CNET, 196 Avenue H. Ravera 92220 BAGNEUX – FRANCE
P. Fremaux
Affiliation:
CNET, 196 Avenue H. Ravera 92220 BAGNEUX – FRANCE
D. Josse
Affiliation:
CNET, 196 Avenue H. Ravera 92220 BAGNEUX – FRANCE
F. Kajzar
Affiliation:
DEIN/LPEM, CEN-SACLAY, 91191 GIF-SUR-YVETTE, CEDEX-FRANCE
J. Zyss
Affiliation:
CNET, 196 Avenue H. Ravera 92220 BAGNEUX – FRANCE
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Abstract

A two-level expression of the second-order hyperpolarizability (y) is proposed, and shown to contain a negative charge transfer (CT) contribution. Frequency dispersed measurements of the quadratic and cubic susceptibility of N-(4-nitropheny1)-L-prolinol (NPP), N-(4-nitrophenyl)-N-methylaminoacetonitrile (NPAN) and 2-(N-prolinol)-5-nitropyridine (PNP) are reported. The electric field induced second-harmonic generation (EFISH) and third-harmonic generation (THG) techniques in solution are used. A two-level model dispersion of y as from THG measurements is shown to lead to a neglegible electronic contribution to the overall EFISH nonlinearity, as compared to the orientational contribution. The theoretical β-components of these molecules, obtained consistently by finite-field and perturbational approaches, clearly confirm that the β-tensor is one-dimensional along the donor-acceptor CT axis. The off resonance quadratic polarizabilities (β) of these molecules are sequenced as follows : β(NPP)> β(PNP)> β(NPAN). However this increased efficiency is obtained at the expense of the transparency range.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 109: Symposium K – Nonlinear Optical Properties of Polymers , 1987 , 171
Copyright
Copyright © Materials Research Society 1988

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References

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