Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.

Recoil-ion and electron momentum spectroscopy is a rapidly developing technique that allows one to measure the vector momenta of several ions and electrons resulting from atomic or molecular fragmentation. In a unique combination, large solid angles close to π Microccopes -the "bubble chambers of atomic physics" -mark the decisive step forward to investigate many-particle quantum-dynamics occurring when atomic and molecular systems or even surfaces and solids are exposed to time-dependent external electromagnetic fields.The present review concentrates on just these latest technical developments and on at least four new classes of fragmentation experiments that have emerged within about the last five years. First, multi-dimensional images in momentum space brought unprecedented information on the dynamics of single-photon induced fragmentation of fixed-in-space molecules and on their structure. Second, a break-through in the investigation of highintensity short-pulse laser induced fragmentation of atoms and molecules has been achieved by using Reaction Microccopes. Third, for electron and ion-impact, the investigation of twoelectron reactions has matured to a state such that first fully differential cross sections (FDCS) are reported. Forth, comprehensive sets of FDCS for single ionisation of atoms by ion-impact, the most basic atomic fragmentation reaction, brought new insight, a couple of surprises and unexpected challenges to theory at keV to GeV collision energies. In addition, a brief summary on the kinematics is provided at the beginning. Finally, the rich future potential of the method is shortly envisaged.2

Bijvoet's method, which makes use of anomalous x-ray diffraction or dispersion, is the standard means of directly determining the absolute (stereochemical) configuration of molecules, but it requires crystalline samples and often proves challenging in structures exclusively comprising light atoms. Herein, we demonstrate a mass spectrometry approach that directly images the absolute configuration of individual molecules in the gas phase by cold target recoil ion momentum spectroscopy after laser ionization-induced Coulomb explosion. This technique is applied to the prototypical chiral molecule bromochlorofluoromethane and the isotopically chiral methane derivative bromodichloromethane.

Quantum theory dictates that upon weakening the two-body interaction in a three-body system, an infinite number of three-body bound states of a huge spatial extent emerge just before these three-body states become unbound. Three helium atoms have been predicted to form a molecular system that manifests this peculiarity under natural conditions without artificial tuning of the attraction between particles by an external field. Here we report experimental observation of this long predicted but experimentally elusive Efimov state of 4 He3 by means of Coulomb explosion imaging. We show spatial images of an Efimov state, confirming the predicted size and a typical structure where two atoms are close to each other while the third is far away. One Sentence Summary:We report experimental discovery of a gigantic molecule that consists of three helium atoms and is bound solely by a universal feature of quantum mechanics called "Efimov effect".Ever since the early days of celestial mechanics, the three-body problem posed a major challenge to physicists. In the early 20th century the failure of finding a stable solution for the classical helium atom (2 electrons and a nucleus) heralded the demise of Niels Bohr's program of semiclassical atomic physics (1). Quantum mechanics then added yet another surprising twist to the three-body problem when in 1970 Vitaly Efimov predicted the appearance of an infinite series of stable three-body states of enormous spatial extents (2). These Efimov states are predicted to exist for short-range interactions like the van der Waals force between atoms or the strong force between nucleons. When the potential becomes so shallow that the last two-body bound state is at the verge of becoming unbound or is unbound, then three particles stick together to form Efimov states. Intriguingly, this three-body behavior does not depend on the details of the underlying two-body interactions. This makes the Efimov effect a universal phenomenon, with important applications in particle, nuclear (3, 4), atomic (4), condensed matter (5) and biological physics (6).Figure 1 summarizes two facets of Efimov's prediction, namely the energy spectrum and the structure of an Efimov state. Figure 1A shows how the two-and three-body binding energies (the binding energy of an atomic cluster is defined as the energy needed to separate all constituents of the cluster to infinite distances) change as the depth of the two-body potential is increased. As 2 indicated by the arrow above Figure 1A, the depth of the two-body potential increases along the horizontal axis. As the depth increases, the s-wave scattering length a changes from negative values to infinitely large values to positive values. Negative a values correspond to the domain where shallow two-body bound states do not exist. For positive a, a shallow two-body bound state, the dimer (see the blue solid line), exists. Bound three-body states (called trimers) exist in the green-shaded area. The extremely weakly-bound three-body states close to threshold (see...

While, at the same time, the correlated momenta of the entangled electron pair continue to exhibit quantum interference.

H 2 , the smallest and most abundant molecule in the universe, has a perfectly symmetric ground state. What does it take to break this symmetry? Here we show that the inversion symmetry can be broken by absorption of a linearly polarized photon, which itself has inversion symmetry.In particular, the emission of a photoelectron with subsequent dissociation of the remaining H + 2 fragment shows no symmetry with respect to the ionic H + and neutral H atomic fragments. This result is the consequence of the entanglement between symmetric and antisymmetric H + 2 states resulting from autoionization. The mechanisms behind this symmetry breaking are general for all molecules.

Although valence electrons are clearly delocalized in molecular bonding frameworks, chemists and physicists have long debated the question of whether the core vacancy created in a homonuclear diatomic molecule by absorption of a single x-ray photon is localized on one atom or delocalized over both. We have been able to clarify this question with an experiment that uses Auger electron angular emission patterns from molecular nitrogen after inner-shell ionization as an ultrafast probe of hole localization. The experiment, along with the accompanying theory, shows that observation of symmetry breaking (localization) or preservation (delocalization) depends on how the quantum entangled Bell state created by Auger decay is detected by the measurement.

We coincidently measure the molecular-frame photoelectron angular distribution and the ion sum-momentum distribution of single and double ionization of CO molecules by using circularly and elliptically polarized femtosecond laser pulses, respectively. The orientation dependent ionization rates for various kinetic energy releases allow us to individually identify the ionizations of multiple orbitals, ranging from the highest occupied to the next two lower-lying molecular orbitals for various channels observed in our experiments. Not only the emission of a single electron, but also the sequential tunneling dynamics of two electrons from multiple orbitals are traced step by step. Our results confirm that the shape of the ionizing orbitals determine the strong laser field tunneling ionization in the CO molecule, whereas the linear Stark effect plays a minor role.