Intermolecular interactions in linear and nonlinear susceptibilities: beyond the local-field approximation

Abstract

Reduced equations of motion for material and radiation field variables in a molecular crystal are presented that allow us to calculate linear- and nonlinear-optical susceptibilities, accounting in a systematic way for intermolecular interactions. These equations are derived starting from the multipolar (μ · D) Hamiltonian, and to second order in the molecular dipole they reduce to the Bloch–Maxwell equations with local-field corrections. The dielectric function obtained through our approach incorporates retarded interactions in a consistent way and is compared with the existing exciton polariton theory, which is based on the minimal coupling (p · A) Hamiltonian. We find that, unlike with the conventional polariton theory, spontaneous emission is not suppressed in an infinite crystal.

© 1989 Optical Society of America

Dielectric response, nonlinear-optical processes, and the Bloch–Maxwell equations for polarizable fluids

Shaul Mukamel, Zhifang Deng, and Jonathan Grad
J. Opt. Soc. Am. B 5(4) 804-816 (1988)

Theoretical and computational aspects of the nonlinear-optical properties of molecules and molecular clusters

Georges H. Wagnière and Jürgen B. Hutter
J. Opt. Soc. Am. B 6(4) 693-702 (1989)

Solvable approximate model for the harmonic radiation from atoms subjected to oscillatory electric fields

L. C. Biedenharn, G. A. Rinker, and Johndale C. Solem
J. Opt. Soc. Am. B 6(2) 221-227 (1989)

Interaction Hamiltonian of quantum optics

J. R. Ackerhalt and P. W. Milonni
J. Opt. Soc. Am. B 1(1) 116-120 (1984)

Material applications of the far-infrared free-electron laser

John D. Simon, John E. Crowell, John H. Weare, and David R. Miller
J. Opt. Soc. Am. B 6(5) 1035-1044 (1989)