Experimental observation of the elusive double-peak structure in R-dependent strong-field ionization rate of H2+

TL;DR

This study experimentally confirms the long-predicted double-peak structure in the R-dependent ionization rate of H2+ molecules, using a pump-probe technique to observe the phenomenon directly for the first time.

Contribution

The paper provides the first experimental observation of the double-peak structure in the R-dependent ionization rate of H2+, validating theoretical predictions.

Findings

Double-peak structure observed in parallel polarization

No double-peak observed in perpendicular polarization

Experiment confirms theoretical models of charge-resonance enhanced ionization

Abstract

When a diatomic molecule is ionized by an intense laser field, the ionization rate depends very strongly on the inter-nuclear separation. That dependence exhibits a pronounced maximum at the inter-nuclear separation known as the critical distance. This phenomenon was first demonstrated theoretically in H2+ and became known as charge-resonance enhanced ionization (CREI, in reference to a proposed physical mechanism) or simply enhanced ionisation (EI). All theoretical models of this phenomenon predict a double-peak structure in the R-dependent ionization rate of H2+. However, such double-peak structure has never been observed experimentally. It was even suggested that it is impossible to observe due to fast motion of the nuclear wavepackets. Here we report a few-cycle pump-probe experiment which clearly resolves that elusive double-peak structure. In the experiment, an expanding H2+ ion produced by an intense pump pulse is probed by a much weaker probe pulse. The predicted double-peak structure is clearly seen in delay-dependent kinetic energy spectra of protons when pump and probe pulses are polarized parallel to each other. No structure is seen when the probe is polarized perpendicular to the pump.