We report on a direct method to measure the interatomic potential energy curve of diatomic systems. A cold target recoil ion momentum spectroscopy reaction microscope was used to measure the squares of the vibrational wave functions of H_{2}, He_{2}, Ne_{2}, and Ar_{2}. The Schrödinger equation relates the curvature of the wave function to the potential V(R) and therefore offers a simple but elegant way to extract the shape of the potential.

Understanding electron-electron correlations in matter ranging from atoms to solids represents a grand challenge for both experiment and theory. These correlations occur on attosecond timescales and have only recently become experimentally accessible. In the case of highly excited systems, the task of understanding and probing correlated interactions is even greater. In this work, we combine state-of-the-art light sources and advanced detection techniques with ab initio calculations to unravel the role of electron-electron correlation in D2 photoionization by mapping the dissociation of a highly excited D2+ molecule. Correlations between the two electrons dictate the pathways along which the molecule dissociates and lead to a superposition of excited ionic states. Using 3D Coulomb explosion imaging and electron-ion coincidence techniques, we assess the relative contribution of competing parent ion states to the dissociation process for different orientations of the molecule with respect to the laser polarization, which is consistent with a shake-up ionization process. As a step toward observing coherent superposition experimentally, we map the relevant nuclear potentials using Coulomb explosion imaging and show theoretically that such an experiment could confirm this coherence via two-path interference.

We have conducted an experimental study on the photo double ionization (PDI) of carbon dioxide dimers and oxygen dimers, while focusing on the dissociation dynamics upon single photon absorption. The results in terms of the kinetic energy and angular distributions of the charged particles show unambiguous experimental evidence of intermolecular Coulombic decay (ICD) in carbon dioxide dimers. In the oxygen dimer, the results show that ICD is accompanied by knock-off ionization mechanisms.

We investigate interatomic Coulombic decay in NeKr dimers after neon inner-valence photoionization [Ne⁺(2s^-1)] using a synchrotron light source. We measure with high energy resolution the two singly charged ions of the Coulomb-exploding dimer dication and the photoelectron in coincidence. By carefully tracing the post-collision interaction between the photoelectron and the emitted ICD electron we are able to probe the temporal evolution of the state as it decays. Although the ionizing light pulses are 80 picoseconds long, we determine the lifetime of the intermediate dimer cation state and visualize the contraction of the nuclear structure on the femtosecond time scale.

We demonstrate the use of cold target recoil ion momentum spectroscopy to perform state-selective measurements of the dissociative channels following single-photon double-ionization of H2O. The two dominant dissociation channels observed lead to two-body (OH++H++2e-) and three-body (2H++O+2e-) ionic fragmentation channels. In the two-body case we observe the presence of an autoionization process with a double-differential cross section that is similar to the single-photon double-ionization of helium well above threshold. In the three-body case, momentum and energy correlation maps in conjunction with new classical trajectory calculations in the companion theory paper by Z. L. Streeter et al. [Phys. Rev. A 98, 053429 (2018)10.1103/PhysRevA.98.053429] lead to the determination of the eight populated dication states and their associated fragmentation geometry. For the latter case, state-specific relative cross sections, median kinetic energy releases, and median angles between asymptotic proton momenta are presented. This benchmark-level experiment demonstrates that, in principle, state-selective fixed-frame triple-differential cross sections can be measured for some dication states of the water molecule.

We have conducted an experimental study on the photo double ionization (PDI) of carbon-dioxide dimers at photon energies of 37 and 55 eV and oxygen dimers at photon energies of 38, 41.5, and 46 eV, while focusing on the dissociation dynamics upon single-photon absorption. The investigation was performed by applying the cold-target recoil-ion momentum spectroscopy method in order to collect and record the three-dimensional momenta of the ionic fragments and emitted electrons from the dissociating dimer in coincidence. The kinetic-energy release upon fragmentation and the electron angular distributions in the laboratory and body-fixed frames, as well as the relative electron-electron emission angle, show unambiguous experimental evidence of intermolecular Coulombic decay (ICD) in carbon-dioxide dimers upon photoionization below and above the double-ionization threshold of CO2 monomers. The PDI of oxygen dimers is less conclusive and shows contributions from ICD and knock-off ionization mechanisms. As for atomic dimers, the present results reveal that ICD in CO2 dimers after valence PDI can also serve as a source for low-energy electrons, known to be very relevant in biological systems, cells, and tissues.