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

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 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.