Abstract
In this chapter we give an introduction to the theory of linear and nonlinear optics. We show how the response of a molecule to an external oscillating electric field can be described in terms of intrinsic properties of the molecules, namely the (hyper)polarizabilities. We outline how these properties are described in the case of exact states by considering the time-development of the exact state in the presence of a time-dependent electric field. Approximations introduced in theoretical studies of nonlinear optical properties are introduced, in particular the separation of electronic and nuclear degrees of freedom which gives rise to the partitioning of the (hyper)polarizabilities into electronic and vibrational contributions. Different approaches for calculating (hyper)polarizabilities are discussed, with a special focus on the electronic contributions in most cases. We end with a brief discussion of the connection between the microscopic responses of an individual molecule to the experimentally observed responses from a molecular ensemble
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References
Baranowska, A., Sadlej, A.J.: Chem. Phys. Lett., 398, 270 (2004)
Bartlett, R.J., Sekino, H.: In Karna, S.P., Yeates, A.T., (eds) Nonlinear Optical Materials, ACS Symposium Ser. 628, p. 23. American Chemical Society, Washington (1996)
Bishop, D.M.: Rev. Mod. Phys., 62, 343 (1990)
Bishop, D.M.: Adv. Quantum Chem., 25, 1 (1994)
Bishop, D.M.: J. Chem. Phys., 100, 6535 (1994)
Bishop, D.M.: Adv. Chem. Phys., 104, 1 (1998)
Bishop, D.M., Cheung, L.M., Buckingham, A.D.: Mol. Phys., 41, 1225 (1980)
Bishop, D.M., Hasan, M., Kirtman, B.: J. Chem. Phys., 103, 4157 (1995)
Bishop, D.M., Kirtman, B.: J. Chem. Phys., 95, 2646 (1991)
Bishop, D.M., Kirtman, B.: J. Chem. Phys., 97, 5255 (1992)
Bishop, D.M., Norman, P.: In Nalwa, H.S. (ed.) Handbook of Advanced Electronic and Photonic Materials, Academic, San Diego (2000)
Bishop, D.M., Pipin, J.: J. Chem. Phys., 91, 3549 (1989)
Bishop, D.M., Pipin, J., Cybulski, S.M.: Phys. Rev. A, 43, 4845 (1991)
Bogaard, M.P., Orr, B.J.: In Buckingham, A.D. (ed.) MTP International Review of Science, Physical Chemistry, vol. 2 of 2, Chap 5, p. 149. Butterworth, London (1975)
Born, M., Huang, K.: Clarendon Press, Oxford. Appendix 8 (1954)
Born, M., Oppenheimer, R.: Ann. d. Phys., 84, 457 (1927)
Boyd, R.W.: Nonlinear Optics. 2nd edition Academic, Inc., San Diego (2003)
Brédas, J.L., Adant, C., Tackx, P., Persoons, A.: Chem. Rev., 94, 243 (1994)
Buckingham, A.D.: Adv. Chem. Phys., 12, 107 (1967)
Buckingham, A.D., Orr, B.J.: Quart. Rev., 21, 195 (1967)
Butcher, P.N., Cotter, D.: The elements of nonlinear optics. Cambridge University Press, Cambridge (1990)
Champagne, B., Kirtman, B.: In: Nalwa, H.S., (ed.) Handbook of Advanced Electronic and Photonic Materials. Academic, San Diego (2000)
Christiansen, O., Jørgensen, P., Hättig, C.: Int. J. Quantum Chem., 68, 1 (1998)
Darling, C.L., Schlegel, H.B.: J. Phys. Chem., 98, 5855 (1994)
Diercksen, G.H.F., Roos, B.O., Sadlej, A.J.: Chem. Phys., 59, 29 (1981)
Dykstra, C.E., Liu, S.-Y., Malik, D.J.: Adv. Chem. Phys., 75, 37 (1989)
Feynman, R.P.: Phys. Rev., 56, 340 (1939)
Flytzanis, C.: In Rabin, H., Tang, C.L., (eds) Quantum Electronics, vol. IA, p. 9. Academic, New York (1975)
Franken, P.A., Hill, A.E., Peters, C.W., Weinreich, G.: Phys. Rev. Lett., 7, 118 (1961)
Hasanein, A.A.: Adv. Chem. Phys., 85, 415 (1993)
Helgaker, T., Jørgensen, P., Olsen, J.: Molecular Electronic-Structure Theory, Wiley (2000)
Hellmann, H.: Einführung in die Quantenchemie. Deuticke, Leipzig (1937)
Kirkwood, J.G.: J. Chem. Phys., 2, 351 (1934)
Kirtman, B., Champagne, B.: Int. Rev. Phys. Chem., 16, 389 (1997)
Koch, H., Jørgensen, P.: J. Chem. Phys., 93, 3333 (1990)
Linderberg, J., Öhrn, Y.: Propagators in Quantum Chemistry. Academic, London (1973)
Linderberg, J., Öhrn, Y.: Propagators in Quantum Chemistry. Wiley, Weinheim (2004)
London, F.: J. Phys. Radium, 8, 397 (1937)
Luo, Y., Ågren, H., Jørgensen, P., Mikkelsen, K.V.: Adv. Quantum Chem., 26, 165 (1995)
Luo, Y., Ågren, H., Vahtras, O., Jørgensen, P.: Chem. Phys. Lett., 207, 190 (1993)
Miertuš, S., Scrocco, E., Tomasi, J.: Chem. Phys., 55, 117 (1981)
Mikkelsen, K.V., Dalgaard, E., Swanstrøm, P.: J. Phys. Chem., 91, 3081 (1987)
Nakano, M., Yamaguchi, K.: Trends in Chemical Physics, 5, 87 (1997)
Nerbrant, P.O., Roos, B.O., Sadlej, A.J.: Int. J. Quantum Chem., 15, 135 (1979)
Norman, P., Jonsson, D., Vahtras, O., Ågren, H.: Chem. Phys., 203, 23 (1996)
Olsen, J., Jørgensen, P.: J. Chem. Phys., 82, 3235 (1985)
Onsager, L.: J. Am. Chem. Soc., 58, 1456 (1936)
Oudar, J.L., Chemla, D.S.: J. Chem. Phys., 66, 2664 (1977)
Prasad, P.N., Williams, D.J.: Introduction to nonlinear optical effects in molecules and polymers. Wiley, Inc., New York (1991)
Pulay, P.: Mol. Phys., 18, 473 (1970)
Pulay, P.: In Yarkony, D.R., (ed.) Modern Electronic Structure Theory, p. 1191. World Scientific (1995)
Rinaldi, D., Rivail, J.-L.: Theor. Chim. Acta, 32, 57 (1973)
Ruud, K., Helgaker, T., Bak, K.L., Jørgensen, P., and Jensen, H.J. Aa. J. Chem. Phys., 99, 3847 (1993)
Sadlej, A.J.: Chem. Phys. Lett., 47, 50 (1977)
Shelton, D.P., Rice, J.E.: Chem. Rev., 94, 3 (1994)
Tomasi, J., Persico, M.: Chem. Rev., 94, 2027 (1994)
Wagniére, G.H.: Linear and nonlinear optical properties of molecules. Verlag Helvetica Chimica Acta, Basel (1993)
Ward, J.F.: Rev. Mod. Phys., 37, 1 (1965)
Wolff, J.J., Wortmann, R.: Adv. Phys. Org. Chem., 32, 121 (1999)
Wolinski, K., Hinton, J.F., Pulay, P.: J. Am. Chem. Soc., 112, 8251 (1990)
Woon, D.E., Dunning Jr., T.H.: J. Chem. Phys., 100, 2975 (1994)
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Norman, P., Ruud, K. (2006). Microscopic Theory of Nonlinear Optics. In: Papadopoulos, M.G., Sadlej, A.J., Leszczynski, J. (eds) Non-Linear Optical Properties of Matter. Challenges and Advances in Computational Chemistry and Physics, vol 1. Springer, Dordrecht. https://doi.org/10.1007/1-4020-4850-5_1
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DOI: https://doi.org/10.1007/1-4020-4850-5_1
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