Understanding diatomic molecular dynamics triggered by a few-cycle pulse

Abstract

In strong field physics, complex atomic and molecular motions can be triggered and steered by an ultrashort strong field. With a given pulse as an carrier-envelope form, E(t) = E₀(t) cos(ωt + φ), we established our photon-phase formalism to decompose the solution of a time-dependent Schrödinger equation in terms of photons. This formalism is further implemented into a general analysis scheme that allows extract photon information direct from the numerical solution. The φ-dependence of any observables then can be understood universally as an interference effect of different photon channels. With this established, we choose the benchmark system H₂⁺ to numerically study its response to an intense few-cycle pulse. This approach helps us identify electronic, rovibrational transitions in terms of photon channels, allowing one to discuss photons in the strong field phenomena quantitatively. Furthermore, the dissociation pathways are visualized in our numerical calculations, which help predicting the outcome of dissociation. Guided by this photon picture, we explored the dissociation in a linearly polarized pulse of longer wavelengths (compared to the 800 nm of standard Ti:Saphire laser). We successfully identified strong post-pulse alignment of the dissociative fragments and found out that such alignment exists even for heavy molecules. More significant spatial asymmetry is confirmed in the longer wavelength regime, because dissociation is no longer dominated by a single photon process and hence allowed for richer interference. Besides, quantitative comparison between theory and experiment have been conducted seeking beyond the qualitative features. The discrepancy caused by different experimental inputs allows us to examine the assumptions made in the experiment. We also extend numerical studies to the dissociative ionization of H₂ by modeling the ionization.