Classical mechanisms of recollision and high harmonic generation

Abstract

Thirty years after the demonstration of the production of high laser harmonics through nonlinear laser-gas interaction, high harmonic generation (HHG) is being used to probe molecular dynamics in real time and is realizing its technological potential as a tabletop source of attosecond pulses in the XUV to soft X-ray range. Despite experimental progress, theoretical efforts have been stymied by the excessive computational cost of first-principles simulations and the difficulty of systematically deriving reduced models for the non-perturbative, multiscale interaction of an intense laser pulse with a macroscopic gas of atoms. In this thesis, we investigate first-principles reduced models for HHG using classical mechanics. On the microscopic level, we examine the recollision process—the laser-driven collision of an ionized electron with its parent ion—that drives HHG. Using nonlinear dynamics, we elucidate the indispensable role played by the ionic potential during recollisions in the strong-field limit. On the macroscopic level, we show that the intense laser-gas interaction can be cast as a classical field theory. Borrowing a technique from plasma physics, we systematically derive a hierarchy of reduced Hamiltonian models for the self-consistent interaction between the laser and the atoms during pulse propagation. The reduced models can accommodate either classical or quantum electron dynamics, and in both cases, simulations over experimentally-relevant propagation distances are feasible. We build a classical model based on these simulations which agrees quantitatively with the quantum model for the propagation of the dominant components of the laser field. Subsequently, we use the classical model to trace the coherent buildup of harmonic radiation to its origin in phase space. In a simplified geometry, we show that the anomalously high frequency radiation seen in simulations results from the delicate interplay between electron trapping and higher energy recollisions brought on by propagation effects.