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A general theory of inhomogeneous broadening for nonlinear susceptibilities: the second hyperpolarizability

2008/02/23 by Robert J. Kruhlak, Kruhlak, Robert J., Mark G. Kuzyk +1
Chemistry · Materials Science · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Molecular spectroscopy and chirality #Nonlinear Optical Materials Research #Optics (physics.optics) #Spectroscopy and Quantum Chemical Studies #physics.chem-ph #physics.optics

paper · pdf · doi:10.48550/arxiv.0802.3421

Submitted to IEEE JSTQE

arxiv created 2008/02/23 · openalex publication_date 2008/02/23 · arxiv updated 2009/12/01 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

A general theory of inhomogeneous broadening is rarely applied to nonlinear spectroscopy in lieu of either a simple Lorentzian or Gaussian model. In this work, we generalize all the important third-order nonlinear susceptibility expressions obtained with sum-over state quantum calculations to include Gaussian and stretched Gaussian distributions of Lorentzians. This theory gives a better fit to subtle spectral features - such as the shoulder of the electroabsorption peak, and is a more accurate tool for determining transition moments from spectroscopy experiments.

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