Electronic correlations govern the dynamics of many phenomena in nature, such as chemical reactions and solid state effects, including superconductivity. Such correlation effects can be most clearly investigated in processes involving single atoms. In particular, the emission of two electrons from an atom--induced by the impact of a single photon, a charged particle or by a short laser pulse--has become the standard process for studies of dynamical electron correlations. Atoms and molecules exposed to laser fields that are comparable in intensity to the nuclear fields have extremely high probabilities for double ionization; this has been attributed to electron-electron interaction. Here we report a strong correlation between the magnitude and the direction of the momentum of two electrons that are emitted from an argon atom, driven by a femtosecond laser pulse (at 38 TW cm(-2)). Increasing the laser intensity causes the momentum correlation between the electrons to be lost, implying that a transition in the laser-atom coupling mechanism takes place.

Viscosity measurements of GaInSn eutectic alloys were performed in a homebuilt device for low (9%) and high (95%) relative humidity for shorter (450 min) and longer (1800 min) time periods. At constant exposure time a characteristic increase of viscosity is observed with increasing humidity. For high humidity, high viscosity is obtained after a short time.Assuming that the measured viscosity change is strongly related to the absorption of oxygen, XPS was applied to the chemical and quantitative analysis of differently prepared samples. In all cases, Ga is predominantly oxidized at the surface whereas Ga atoms in the metallic state are located deeper inside. Besides Ga 2 O 3 (the most stable oxide phase), the less stable Ga 2 O is detected. Indium and tin are almost stable in their metallic state. With increasing humidity the thickness of the oxide film increases in our case from about 19Å to 25Å, assuming a layer-by-layer model. The presented results confirm our assumption of the increase in viscosity of the GaInSn system as a consequence of the preferential oxidation of gallium in the near-surface region.

In 1997, it was predicted that an electronically excited atom or molecule placed in a loosely bound chemical system (such as a hydrogen-bonded or van-der-Waals-bonded cluster) could efficiently decay by transferring its excess energy to a neighbouring species that would then emit a low-energy electron. This intermolecular Coulombic decay (ICD) process has since been shown to be a common phenomenon, raising questions about its role in DNA damage induced by ionizing radiation, in which low-energy electrons are known to play an important part. It was recently suggested that ICD can be triggered efficiently and site-selectively by resonantly core-exciting a target atom, which then transforms through Auger decay into an ionic species with sufficiently high excitation energy to permit ICD to occur. Here we show experimentally that resonant Auger decay can indeed trigger ICD in dimers of both molecular nitrogen and carbon monoxide. By using ion and electron momentum spectroscopy to measure simultaneously the charged species created in the resonant-Auger-driven ICD cascade, we find that ICD occurs in less time than the 20 femtoseconds it would take for individual molecules to undergo dissociation. Our experimental confirmation of this process and its efficiency may trigger renewed efforts to develop resonant X-ray excitation schemes for more localized and targeted cancer radiation therapy.

High resolution laser excitation was combined with the technique of mass-selected two-photon ionization via aresonant intermediate state to measure rotationally resolved UV spectra of benzene-Ar van der Waals clusters. When the second laser pulse in the two color experiment is delayed by 7 ns no line broadening due to the second ionizing absorption step is observed. Spectra of three vibronic bands in the SI +-So transition ofbenzene (h 6 )-Ar and benzene (d 6 )-Ar were measured yielding a line spectrum with a linewidth of 130 MHz. Resolution is sufficient to demonstrate that no asymmetry splitting of the rotationallines occurs and the spectrum is to a high precision that of a symmetrie rotor. A detailed analysis ofthe rotational structure yields an accurate set ofrotational constants. We find that the Ar is located on the C 6 rotational axis. Its distance from the benzene ring plane is 3.582 A in the electronic ground state and decreases by 59 ± 3 mA in the electronically excited state due to the increased polarizability of the benzene moleeule after electronic excitation.

We present kinematically complete measurements of the photo double ionization of ethylene (double CC bond) and acetylene (triple CC bond) hydrocarbons just above the double ionization threshold. We discuss the results in terms of the coincident kinetic energy of the photo electrons and the nuclear kinetic energy release of the recoiling ions. We have incorporated quantum chemistry calculations to interpret which of the electronic states of the dication have been populated and trace the various subsequent fragmentation channels. We suggest pathways that involve the electronic ground and excited states of the precursor ethylene dication and explore the strong influence of the conical intersections between the different electronic states. The nondissociative ionization yield is small in ethylene and high in acetylene when compared with the dissociative ionization channels.The reason for such a striking difference is explained in part on the basis of a propensity rule which influences the population of states in the photo double ionization of a centrosymmetric closed shell molecule by favoring singlet ungerade and triplet gerade final states. This propensity rule and the calculated potential energy surfaces clarify a picture of the dynamics leading to the observed dication dissociation products.