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Quantum Chemical Methods for the Design of Molecular Non-Linear Optical Materials

Published online by Cambridge University Press:  15 February 2011

Stephen Till  and
Jennifer Till
Stephen Till
Affiliation:
Defense Research Agency, Malvern, Worcs. WR14 3PS, UK
Jennifer Till
Affiliation:
Defense Research Agency, Malvern, Worcs. WR14 3PS, UK
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Abstract

The quantum chemical design of new molecular materials for non-linear applications requires a fundamental understanding of electronic structure and properties. Targeted synthesis of candidates greatly reduces the costs and timescales of an empirical search and this is aided by prior calculation of excited state energies, energy relaxation and transfer rates, molecule-environment interactions and excited state chemistry.

Essentially, the problems encountered in the routine application of standard quantum chemical methods are caused by the large size of the molecules of interest. This necessitates either the design of ultra-fast computers or numerical methods which facilitate the application of ‘exact’ techniques or the development of less resource intensive approximate methods with proven accuracy.

We shall outline the theories used in the calculation of optical properties and review their computational implementation. Calculations on annellated tetraazaporphyrazines will be presented in illustration.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 374: Symposia ZB – Materials for Optical Limiting , 1994 , 3
Copyright
Copyright © Materials Research Society 1995

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References

1 McWeeny, R. and Sutcliffe, B.T., ‘Methods of Molecular Quantum Mechanics’, Academic Press (1969).Google Scholar
2 Roothaan, C.C.J., Rci.Mod.Phys., 23, 69 (1951).Google Scholar
3 Boys, S.F., Proc.Roy.Soc., A200, 542 (1950).Google Scholar
4 Hückel, E., Z.Phys., 70, 204 (1931).Google Scholar
5 Pople, J.A., Trous.Farad.Soc. 49, 1375 (1953).Google Scholar
6 Pariser, R. and Parr, R., J.Chem.Phys., 21, 466,767 (1953).Google Scholar
7 Mataga, N. and Nishimoto, K., Z.Phys.Chem., 13, 140 (1957).Google Scholar
8 Ohno, K., ‘Notes on Molecular Orbital Calculations of ir-electron Systems’, Quantumn Chemistry Group, Uppsala (1963).Google Scholar
9 Griffiths, J., Dyes and Pigments, 3, 211 (1982).Google Scholar
10 Pople, J.A. and Segal, G.A., J.Chem.Phys., 44, 3289 (1966).Google Scholar
11 Pople, J.A., Santry, D.P. and Segal, G.A., J.Chem.Phys., 43, S129 (1965).Google Scholar
12 Pople, J.A., Beveridge, D.L. and Dobosch, P.A., J.Chem.Phys., 47, 2026 (1967).Google Scholar
13 Kotzian, M.. Rösch, N., Schröder, H. and Zerner, M.C., J.Am.Chem.Soc., 111, 7687 (1989) and references therein.Google Scholar
14 Stewart, J.J.P., J.Compul.Chem., 10, 209 (1989).Google Scholar
15 Pople, J.A. et al., Gaussian Inc., Pittsburgh, PA (1992).Google Scholar
16 Dupuis, M. el al in ‘Mod. Tech. in Comp. Chem. : MOTECC 90’, ed. Clementi, E., ESCOM, Leiden (1990).Google Scholar
17 Stanton, J.F. et al, Quantum Theory Project, University of Florida.Google Scholar
18 Huke, J.P., Parsons, l.W. and Till, S.J., J.Chem.Phys. 93, 1814 (1990).Google Scholar
19 Baerends, E.J., Ellis, D.E. and Ros, P., J.Chem.Phys., 2, 41 (1973).Google Scholar
20 Mcllugh, A.J., Gouterman, M. and Weiss, C., Theorat. Chimica Acta, 24, 346 (1972).Google Scholar
21 Till, J. and Till, S. J., DRA Memorandum 4783 (1993).Google Scholar
22 Slater, J.C.. “The Self Consistenm Field for Molecules and Solids: Quantum Theory of Molecuiles and Solids, Vol.IV’, McGraw-Hill (1968).Google Scholar
23 Gouterman, M.. Wagniere, G.H. and Snyder, L.C., J.Mol.Spcetrosc., 11, 1108 (1963).Google Scholar
24 migold, C.K., ‘Structure and Mechanism in Organic Chemistry’, Bell (1969).Google Scholar
25 Dvornikov, S.S.. Knyukslito, V.N., Kuzmiitsky, V.A., Shulga, A.M. and Solovyov, K.N., J. Luminescouse, 23, 373 (1981).Google Scholar
26 Vincent, P.S., Voigl, E.M. and Rieckhoff, K.E., J.Chem.Phys., 55,4131 (1971).Google Scholar
27 Till, S.J.. Howard, S.T. and Parsons, I.W., J.Chem.Phys., 95, 9079 (1991).Google Scholar
28 Welford, K.R.. Hollins, R.C., McEwan, K.J., Till, S.J. and Swatton, S.N.R., these procecdingsGoogle Scholar