Extracting Information on Linear and Nonlinear Absorption from Two-Beam Action Spectroscopy Data.

Two-beam action (2-BA) spectroscopies are a recently developed class of techniques for determining the order(s) of absorption (one-photon, two-photon, etc.) that contribute to an observable signal. When only a single order of absorption is present, 2-BA spectroscopies allow for the determination of that order from data obtained at a single value of the observable. It has been shown previously that when two orders of absorption are present, they can be determined unambiguously from measurements made at several values of the observable. However, this latter approach cannot be used for single-valued observables, such as a polymerization threshold. Here we develop a theoretical comparison between conventional methods that determine the order(s) of absorption using logarithmic plots and 2-BA-based techniques. We also explore how 2-BA plots arising from two orders of absorption deviate from a plot with a single, noninteger exponent. We demonstrate that these deviations can usually be used to identify the two orders of absorption and their relative contributions to the signal on the basis of measurements made at a single value of the observable.