Three-wave mixing in chiral liquids

Year: 2000

Authors: Fischer P., Wiersma D., Righini R., Champagne B., Buckingham AD.

Autors Affiliation: Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom; Europ. Lab. for Nonlinear Spectrosc., Largo E. Fermi 2, 50125 Florence, Italy; Ist. Naz. per la Fis. della Materia, Largo E. Fermi 2, 50125 Florence, Italy; FUNDP, Lab. de Chim. Theor. Appl., rue Bruxelles 61, B-5000 Namur, Belgium

Abstract: Second-order nonlinear optical frequency conversion in isotropic systems is only dipole allowed for sum- and difference-frequency generation in chiral media. We develop a single-center chiral model of the three-wave mixing (sum:frequency generation) nonlinearity and estimate its magnitude. We also report results from ab initio calculations and from three- and four-wave mixing experiments in support of the theoretical estimates. We show that the second-order susceptibility in chiral liquids is much smaller than previously thought.

Journal/Review: PHYSICAL REVIEW LETTERS

Volume: 85 (20)      Pages from: 4253  to: 4256

KeyWords: Electron transitions; Electronic density of states; Estimation; Four wave mixing; Ground state; Liquids; Magnetic moments; Mathematical models; Molecular vibrations; Optical frequency conversion; Optical properties; Second harmonic generation, Absorption band; Chiral liquids; Electric dipole transition matrix element; Isotropic systems; Magnetic dipole transition moment; Molecular chirality; Supramolecular chiral clusters; Three wave mixing, Molecular physics
DOI: 10.1103/PhysRevLett.85.4253

Citations: 112
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