Non-perturbative Effects in Attosecond Four-Wave Mixing Spectra

TL;DR

This paper investigates the nonlinear optical response of argon in attosecond four-wave mixing, revealing non-perturbative effects and state couplings through combined experimental measurements and ab initio simulations.

Contribution

It provides the first detailed analysis of non-perturbative effects in attosecond four-wave mixing spectra involving autoionizing states.

Findings

Double-peak delay dependence structure observed and simulated.

Rabi cycling causes destructive interference at the signal minimum.

Excellent agreement between experimental data and ab initio simulations.

Abstract

We study the nonlinear optical response of argon to a four-wave-mixing pulse sequence consisting of an extreme ultraviolet pulse, an overlapping collinear IR and an non-collinear delayed IR pulses. Absorption of an extreme ultraviolet and an IR photon from the collinear beams excites, sequentially, the $3s^{-1}4p$ bright state and the {$3s^{-1}3d/5s$} dark states. The subsequent absorption of an IR photon from the non-collinear beam results in an angled extreme ultraviolet emission whose variation with delay encodes coupling between autoionizing-states, dark-state lifetimes, and non-perturbative effects. Both our measurements and \emph{ab initio} simulations of the angled four-wave-mixing signal show a double-peak structure in delay dependence, in excellent agreement with each other. We attribute the minimum at the center of the signal to the rapid Rabi cycling, driven by the IR pulse, between dark states and the $3s^{-1}4p$ resonance, which results in the destructive interference in the final transition amplitude.