Self-Consistent Approach for Simplifying the Molecular Interpretation of Nonlinear Optical and Multiphoton Phenomena
- 29 January 2005
- journal article
- research article
- Published by American Chemical Society (ACS) in The Journal of Physical Chemistry A
- Vol. 109 (7), 1316-1323
- https://doi.org/10.1021/jp045866w
Abstract
A method is developed for simplifying molecular interpretations of nonlinear optical phenomena. General sum-over-states expressions derived from perturbation theory can be written identically and self-consistently as simple products of lower-order effects. Electric dipole-allowed expressions for the nonlinear polarizability reduce to straightforward formulas directly connected to intuitive molecular properties without sacrificing mathematical rigor. This approach is sufficiently general to allow its application in treating electronic, vibrational, and vibronic interactions for both parametric (passive) processes (e.g., wave-mixing spectroscopies, sum- and difference-frequency generation, harmonic generation, etc.) and nonparametric (active) processes (e.g., hyper-Raman spectroscopy, multiphoton absorption, etc.). Explicit examples for sum-frequency generation and for four-wave mixing provide a convenient context for interpreting higher order nonlinear optical processes.Keywords
This publication has 24 references indexed in Scilit:
- Chirality and polarization effects in nonlinear opticsJournal of Optics A: Pure and Applied Optics, 2004
- Polarizability and the resonance scattering of light: Damping sign issuesPhysical Review A, 2003
- Influence of damping on the vanishing of the linear electro-optic effect in chiral isotropic mediaPhysical Review A, 2003
- Reply to “Comment on ‘Phenomenological damping in optical response tensors’ ”Physical Review A, 2001
- Comment on “Phenomenological damping in optical response tensors”Physical Review A, 2001
- Phenomenological damping of nonlinear-optical response tensorsPhysical Review A, 1998
- Selection rules for optical activity and linear birefringence bilinear in electric and magnetic fieldsJournal of Physics B: Atomic, Molecular and Optical Physics, 1989
- Nonlinear atomic susceptibilitiesJournal of Physics B: Atomic and Molecular Physics, 1976
- Studies of nonlinear phenomena - I. Theory of the hyper Raman effectProceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, 1970
- Calculation of Nonlinear Optical Susceptibilities Using Diagrammatic Perturbation TheoryReviews of Modern Physics, 1965