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

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 H-2(+) and became known as charge-resonance enhanced ionization (CREI, in reference to a proposed physical mechanism) or simply enhanced ionization(EI). All theoretical models of this phenomenon predict a double-peak structure in the R-dependent ionization rate of H-2(+). 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 H-2(+) 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.