Nonlinear photoconductivity in pump-probe spectroscopy. I. Optical coefficients

Abstract: We analyze the optical pump-probe reflection and transmission coefficients when the photoinduced response depends nonlinearly on the incident pump intensity. Under these conditions, we expect the photoconductivity depth profile to change shape as a function of the incident fluence, unlike the case when the photoinduced response is linear in the incident intensity. We consider common optical nonlinearities, including photoconductivity saturation and two-photon absorption, and we derive analytic expressions for the photoconductivity depth profile when one or more is present. We review the theory of the electromagnetic transmission and reflection coefficients in a stratified medium, and we derive general expressions for these coefficients for a medium with an arbitrary photoconductivity depth profile. For several photoconductivity profiles of importance in pump-probe spectroscopy, we show that the wave equation can be transformed into one of three standard differential equations$\unicode{x2014}$the Bessel equation, the hypergeometric equation, and the Heun equation$\unicode{x2014}$with analytic solutions in terms of their associated special functions. From these solutions, we derive exact analytic expressions for the optical coefficients in terms of the photoconductivity at the optical interface, and we discuss their limiting forms in various physical limits. Our results provide a systematic guide for analyzing pump-probe measurements over a wide range of pump intensities, and establishes a framework for constraining the systematic uncertainty associated with nonlinear photoconductivity profile distortion.