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

TL;DR

This study demonstrates CEP-controlled electron localization in H2+ photodissociation using ultrashort laser pulses, with experimental results aligning closely with advanced theoretical calculations, revealing fundamental control mechanisms.

Contribution

It provides the first direct measurement of CEP effects on electron localization in molecular ion dissociation without prior ionization influence.

Findings

CEP controls electron localization during dissociation

Experimental data matches ab initio 3D-TDSE calculations

No prior ionization influences the CEP dependence

Abstract

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.