2008/02/23 by Robert J. Kruhlak, Kruhlak, Robert J., Mark G. Kuzyk +1
Engineering · Materials Science · Physics and Astronomy · #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Nonlinear Optical Materials Research #Nonlinear Optical Materials Studies #Optics (physics.optics) #Spectroscopy and Quantum Chemical Studies #physics.chem-ph #physics.optics
paper · pdf · doi:10.48550/arxiv.0802.3420
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
While nonlinear optical spectroscopy is becoming more commonly used to study the excited states of nonlinear-optical systems, a general theory of inhomogeneous broadening is rarely applied in lieu of either a simple Lorentzian or Gaussian model. In this work, we generalize all the important linear and second-order nonlinear susceptibility expressions obtained with sum-over state quantum calculations to include Gaussian and stretched Gaussian distributions of Lorentzians. We show that using the correct model to analyze experiments that probe a limited wavelength range can be critical and that this theory is better able to fit the subtle spectral features - such as the shoulder region of a resonance - when both models produce qualitatively similar responses.