Coherent control at its most fundamental: CEP-dependent electron localization in photodissoziation of a H2+ molecular ion beam target

Measurements and calculations of the absolute carrier-envelope phase (CEP) effects in the photodissociation of the simplest molecule, H2+, with a 4.5-fs Ti:Sapphire laser pulse at intensities up to (4 +- 2)x10^14 Watt/cm^2 are presented. Localization of the electron with respect to the two nuclei (during the dissociation process) is controlled via the CEP of the ultra-short laser pulses. In contrast to previous CEP-dependent experiments with neutral molecules, the dissociation of the molecular ions is not preceded by a photoionization process, which strongly influences the CEP dependence. Kinematically complete data is obtained by time- and position-resolved coincidence detection. The phase dependence is determined by a single-shot phase measurement correlated to the detection of the dissoziation fragments. The experimental results show quantitative agreement with ab inito 3D-TDSE calculations that include nuclear vibration and rotation.Comment: new version includes minore changes and adding the supp_material.pd

Manipulating ionization path in a Stark map: Stringent schemes for the selective field ionization in highly excited Rb Rydberg atoms

We have developed a quite stringent method in selectivity to ionize the low angular- momentum ($\ell$) states which lie below and above the adjacent manifold in highly excited Rb Rydberg atoms. The method fully exploits the pulsed field-ionization characteristics of the manifold states in high slew-rate regime: Specifically the low $\ell$ state below (above) the adjacent manifold is firstly transferred to the lowest (highest) state in the manifold via the adiabatic transition at the first avoided crossing in low slew-rate regime, and then the atoms are driven to a high electric field for ionization in high slew-rate regime. These extreme states of the manifold are ionized at quite different fields due to the tunneling process, resulting in thus the stringent selectivity. Two manipulation schemes to realize this method actually are demonstrated here experimentally.Comment: 10 pages, 4 figure

Systematic observation of tunneling field-ionization in highly excited Rb Rydberg atoms

Pulsed field ionization of high-$n$ (90 $\leq n \leq$ 150) manifold states in Rb Rydberg atoms has been investigated in high slew-rate regime. Two peaks in the field ionization spectra were systematically observed for the investigated $n$ region, where the field values at the lower peak do not almost depend on the excitation energy in the manifold, while those at the higher peak increase with increasing excitation energy. The fraction of the higher peak component to the total ionization signals increases with increasing $n$, exceeding 80% at $n$ = 147. Characteristic behavior of the peak component and the comparison with theoretical predictions indicate that the higher peak component is due to the tunneling process. The obtained results show for the first time that the tunneling process plays increasingly the dominant role at such highly excited nonhydrogenic Rydberg atoms.Comment: 8 pages, 5 figure

Line-narrowing transient Raman technique which resolves closely spaced hydrogen-bonded aggregates

An ultrafast coherent Raman spectroscopy with tunable excitation is presented. It is applied to the analysis of vibrational spectra of hydrogen-bonded aggregates of pyridine and methanol. Whereas the spontaneous Raman spectrum exhibits a broad and featureless band, the line-narrowed spectra reveal three distinct lines. The concentration dependence of these lines suggests an assignment to well-defined aggregates of different sizes