Simultaneous probing of geometry and electronic orbital of ArCO by Coulomb-explosion imaging and angle-dependent tunneling rates

Abstract

We simultaneously probe the molecular structure and the symmetry of valence electronic orbital of an anisotropic atomic-molecular complex of ArCO by tracing its three-body Coulomb breakup following triple ionization in a phase-controlled elliptically polarized two-color pulse. The geometry of ArCO is found to be tilted T shaped, where the angle between the covalent and van der Waals bonds is 65\ifmmode^\circ\else\textdegree\fi{} with oxygen pointing towards argon. The asymmetric profiles of the outmost orbitals from the CO site are probed by directional dissociation of the contained CO subunit as a function of the laser phase. Our results clearly image the asymmetric geometry of ArCO and thus reveal the anisotropic interaction between a rare-gas atom and a heteronuclear diatomic molecule.