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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.

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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

REFERENCES

[1] Armstrong, J.A., Bloembergen, N., Ducuing, J. and Pershan, P.S., Phys. Rev., 127 (6), 1918 (1962)Google Scholar
[2] Wa-rd, J.F., Rev. Mod. Phys. 37, 1 (1965)Google Scholar
[3] Kelley, P.L., J. Phys. Chem.olids 24, 607 (1963)CrossRefGoogle Scholar
[4] Nicoud, J.F. and Twieg, R.J., in Nonlinear Optical properties of Organic Molecules and Crystals, Edited by Cnemia, U.S. and Zyss, J. (Academic, Orlando, Fla, 1987) vol.1 Google Scholar
[5] Oudar, J.L. and Chemla, D.S., J. Chem. Phys. 66, 2664 (1977)CrossRefGoogle Scholar
[6] Zyss, J., J. Chem. Phys. 71, 909 (1979)Google Scholar
[7] Zyss, J., Nicoud, J. F. and.Coquillay, M., J. Chem. Phys. 81, 4160 (1984)Google Scholar
[8] Twieg, R. J. and Dirck, C. W., J. Chem. Phys. 85, 3537 (1986)Google Scholar
[9] Barzoukas., M. Josse, D., Frémaux, P., Zyss, J.. Nicoud, J. F Morly, J.O. J O S A B 4, 977(1987),CrossRefGoogle Scholar
[10] Oudar, J. L.and Person, H. Le, Opt. Com. 15, 258 (1976)Google Scholar
[11] Ouder, J. L. J Chem phys 67Google Scholar
[12]'Bethea, C. G., Appl.Opt. 14,1447, (1975)Google Scholar
[13] Levine, B. F. and Bethea, C. G., J. Chem. Phys. 65, 2429 (1976)CrossRefGoogle Scholar
[14] Singer, K.D. and Garito, A. F., J. Chem. Phys., 75 3572 (1981)Google Scholar
[15] Ledoux, I. and Zyss, J., Chem. Phys. 73, 203 (19827)Google Scholar
[16] Kajzar, F. and Messier, J., Rev. Sci.Instrum. 58, 2061 (1987)Google Scholar
[17] Bertinelli, F., Palmieri, P., Brillante, A. and Taliani, C., Chem. Phys. 25, 333 (1977)Google Scholar
[18] Danilova, V. I. and Morozava, Yu. P., Opt. Spectrosc. 12, 5 (1962)Google Scholar
[19] Lim, E.C., in Excited States, edited by Lim, E.C (Academic press INC, 1974), Vol. 1 p.196 Google Scholar
[20] Kajzar, F., Ledoux, I., Zyss, J., Phys. Rev. A 36, 2210 (1987)Google Scholar
[21] Kajzar, F., to be publishedGoogle Scholar
[22] Meredith, G. Buchalter, B. and Hanzlik, C., J. Chem. Phys. 78, 1543(1983)Google Scholar
[23] Kajzar, F. and Messier, J., Phys. Rev. A 32, 2352 (1985)Google Scholar
[24] Zyss, J., J. Chem. Phys. 70, 3333 (1979); 70, 3341 (1979)Google Scholar
[25] Docherty, V.J., Pugh, D. andMorley, J.O., J.-Them. Soc. Faraday Trans. 2 81, 1179 (1985)Google Scholar
[26] Blanchard, M.. Ledoux, I., Lehn, J.M., Zyss, J., submitted to Chem. Communications.Google Scholar