Modeling of Nonlinear Optical Response in Gaseous Media and its Comparison with Experiment

Abstract

This thesis demonstrates the model and application of nonlinear optical response with Metastable Electronic State Approach (MESA) in ultrashort laser propagation and verifies accuracy of MESA through extensive comparison with experimental data. The MESA is developed from quantum mechanics to describe the nonlinear off-resonant optical response together with strong-field ionization in gaseous medium. The conventional light-matter interaction models are based on a piece-wise approach where Kerr effect and multi-photon ionization are treated as independent nonlinear responses. In contrast, MESA is self-consistent as the response from freed electrons and bound electrons are microscopically linked. It also can be easily coupled to the Unidirectional Pulse Propagation Equations (UPPE) for large scale simulation of experiments. This work tests the implementation of MESA model in simulation of nonlinear phase transients of ultrashort pulse propagation in a gaseous medium. The phase transient has been measured through Single-Shot Supercontinuum Spectral Interferometry. This technique can achieve high temporal resolution (10$fs$) and spatial resolution (5 $\mu m$). Our comparison between simulation and experiment gives a quantitive test of MESA model including post-adiabatic corrections. This is the first time such a comparison was achieved for a theory suitable for large scale numerical simulation of modern nonlinear-optics experiments. In more than one respect, ours is a first-of-a-kind achievement. In particular, Large amount of data are compared. We compare the data of nonlinear response induced by different pump intensity in Ar and Nitrogen. The data sets are three dimensions including two transverse spacial dimensions and one axial temporal dimension which reflect the whole structure of nonlinear response including the interplay between Kerr and plasma-induced effects. The resolutions of spatial and temporal dimension are about a few micrometer and several femtosecond. The regime of light-matter interaction investigated here is between the strong and perturbative, where the pulse intensity can induce nonlinear refractive index change and partial ionization of dielectric medium. Obviously, such regimes are difficult to study both experimentally and theoretically. MESA is a quantum based model, but it retains the same computation complexity as conventional light-matter interaction model. MESA contains the response from both bound and continuum states in a single self-consistent "Package". So, it is fair to say that this experiment-theory comparison sets a new standard for nonlinear light-matter interaction models and their verification in the area of extreme nonlinear optics.