A general theory of inhomogeneous broadening for nonlinear susceptibilities: polarizability and hyperpolarizability

Details A general theory of inhomogeneous broadening for nonlinear susceptibilities: polarizability and hyperpolarizability A general theory of inhomogeneous broadening for nonlinear susceptibilities: polarizability and hyperpolarizability

2008-02-23

arxiv.org/abs/0802.3420v1

Physics

Optics

Submitted to IEEE JSTQE

Scientific paper

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.

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