Theoretical Chemistry Accounts

, Volume 99, Issue 6, pp 384–390 | Cite as

Calculation of macroscopic first- and third-order optical susceptibilities for the benzene crystal

  • H. Reis
  • S. Raptis
  • M. G. Papadopoulos
  • R. H. C. Janssen
  • D. N. Theodorou
  • R. W. Munn
Regular article

Abstract.

Starting from a set of high-level ab initio frequency-dependent molecular first- and third-order polarizabilities, the macroscopic first-order (linear) and third-order (cubic) susceptibilities of the benzene crystal are calculated. Environmental effects are taken into account using a rigorous local-field theory and are compared with the anisotropic Lorentz field factor approach. The experimentally determined first-order susceptibility of crystalline benzene is accurately reproduced. Dispersion curves for the first-order susceptibility and results for electric-field-induced second-harmonic generation and third-harmonic generation experiments are predicted. Comparison with similar calculations conducted in the course of molecular simulations of liquid benzene shows that the theoretical results for the two phases are of comparable accuracy. Overall, the results show that for the fairly compact nonpolar benzene molecules, environmental effects on the effective molecular response are small.

Key words: Susceptibilities Benzene crystal Polarizabilities Hyperpolarizabilities 

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Copyright information

© Springer-Verlag Berlin Heidelberg 1998

Authors and Affiliations

  • H. Reis
    • 1
  • S. Raptis
    • 1
  • M. G. Papadopoulos
    • 1
  • R. H. C. Janssen
    • 2
  • D. N. Theodorou
    • 2
  • R. W. Munn
    • 3
  1. 1.Institute of Organic and Pharmaceutical Chemistry, National Hellenic Research Foundation, Vasileos Constantinou 48, GR-11635 Athens, GreeceGR
  2. 2.Department of Chemical Engineering, University of Patras and Institute of Chemical Engineering and High Temperature Chemical Processes, GR-26500 Patras, GreeceGR
  3. 3.Department of Chemistry, UMIST, Manchester M60 1QD, UKGB

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