Exploring interatomic Coulombic decay by free electron lasers

To exploit the high intensity of laser radiation, we propose to select frequencies at which single-photon absorption is of too low energy and two or more photons are needed to produce states of an atom that can undergo interatomic Coulombic decay (ICD) with its neighbors. For Ne(2) it is explicitly demonstrated that the proposed multiphoton absorption scheme is much more efficient than schemes used until now, which rely on single-photon absorption. Extensive calculations on Ne(2) show how the low-energy ICD electrons and Ne(+) pairs are produced for different laser intensities and pulse durations. At higher intensities the production of Ne(+) pairs by successive ionization of the two atoms becomes competitive and the respective emitted electrons interfere with the ICD electrons. It is also shown that a measurement after a time delay can be used to determine the contribution of ICD even at high laser intensity.     

Electron-transfer-mediated decay and interatomic Coulombic decay from the triply ionized states in argon dimers

We report the first observation of electron-transfer-mediated decay (ETMD) and interatomic Coulombic decay (ICD) from the triply charged states with an inner-valence vacancy, using the Ar dimer as an example. These ETMD and ICD processes, which lead to fragmentation of Ar(3+)-Ar into Ar(2+)-Ar(2+) and Ar(3+)-Ar+, respectively, are unambiguously identified by electron-ion-ion coincidence spectroscopy in which the kinetic energy of the ETMD or ICD electron and the kinetic energy release between the two fragment ions are measured in coincidence.     

Properties of resonant interatomic Coulombic decay in Ne dimers

Properties of the interatomic Coulombic decay (ICD) process in Ne dimers have been obtained by tracking the formation of energetic Ne+ ions. The double photoionization cross section, deduced from the Ne+/Ne+ coincidence signal, is dominated by the ICD process and presents a threshold 280 meV below the atomic Ne+2s(-1) threshold. Rydberg excitation of a 2s electron in the dimer creates molecular Rydberg states whose Sigma and Pi symmetries have been resolved. These excited states decay by a resonant ICD process releasing an energetic Ne+ ion and a neutral excited Ne* fragment. Subsequent autoionization of the Ne* fragment explains a double photoionization threshold below the dimer 2s ionization threshold.     

Femtosecond interatomic Coulombic decay in free neon clusters: large lifetime differences between surface and bulk

A quantitative determination of 2s vacancy lifetimes in surface and bulk atoms of free Ne clusters has been made. While for free atoms the 2s inner-valence hole has a ps lifetime, it reduces to 6+/-1 fs for cluster bulk atoms. For surface atoms, the lifetime is on average longer than 30 fs. The lifetime estimate was obtained from fits of high-resolution photoelectron spectra of Ne clusters. The shortening of the lifetime is attributed to the coordination dependent interatomic Coulombic decay, which is extremely sensitive to internuclear distances.     

Doppler-free resonant Raman auger spectroscopy of Ne+ 2s2p(5)3p excited states

Using very high resolution achieved by the Doppler-free resonant Raman Auger technique, we have resolved the lowest terms of the series of inner-valence excitations 2s2p(5)((1,3)P)np 2S, 2P, and 2D in Ne+. The measured Auger anisotropic parameters and branching ratios help to establish the assignments of these levels. The measured lifetime widths are in reasonable agreements with ab initio calculations available in the literature.     

Theoretical calculation of triple differential cross sections of 3s orbital of argon in coplanar symmetric （e, 2e） reaction

The triple differential cross section for the low-energy electron impact ionization of inner-valence 3s orbital of argon has been calculated using the modified distorted wave Born approximation in coplanar symmetric energy-sharing geometry. Satisfactory agreement between theory and experiraent is achieved when the polarization and post-collisional interaction (PCI) are included in the calculations. It is shown that the polarization and PCI effects play a very important role in the case of argon at low incident energies.     

Three-electron interatomic Coulombic decay from the inner-valence double-vacancy states in NeAr

We have unambiguously identified interatomic Coulombic decay in NeAr from the inner-valence double-vacancy state Ne-Ar(2+)(3s(-2)) to outer-valence triple-vacancy states Ne(+)(2p(-1))-Ar(2+)(3p(-2)) by momentum-resolved electron-ion multicoincidence. This is the first observation of interatomic Coulombic decay where three electrons (3e) participate. The results suggest that this 3e interatomic Coulombic decay is significantly faster than other competing processes like fluorescence decay and charge transfer via curve crossing.     

Experimental observation of interatomic coulombic decay in neon dimers

Recently Cederbaum et al. [Phys. Rev. Lett. 79, 4778 (1997)]] predicted a new decay channel of excited atoms and molecules termed interatomic Coulombic decay (ICD). In ICD the deexcitation energy is transferred via virtual photon exchange to a neighboring atom, which releases it by electron emission. We report on an experimental observation of ICD in 2s ionized neon dimers. The process is unambiguously identified by detecting the energy of two Ne1+ fragments and the ICD electron in coincidence, yielding a clean, background free experimental spectral distribution of the ICD electrons.     

Ionization and electron capture in neon K vacancy production from NNe collisions

Our measurements of Ne K and N K X-ray cross sections for N^{3+,4+,5+,6+,7+,} ions incident on a thin Ne target at energies from 9 to 54 MeV indicate that charge exchange plays a minor role compared to ionization in producing Ne K vacancies over that energy range.     

On the mechanism of the reactions24,25,26Mg(n,α)21,22,23Ne at neutron energies near 14 MeV

Differential cross sections of the reactions²⁴Mg(n,α)²¹Ne,²⁵Mg(n,α)²²Ne, and²⁶Mg(n,α)²³Ne have been measured at neutron energies of 13.19,13.93 and 14.33 MeV, at 13.93 and 14.33 MeV, and at 13.47 and 13.93 MeV, respectively. In forward direction, differential excitation functions of those reactions have been measured at energies between 12.67 and 16.05 MeV. The results are analysed in terms of direct-reaction and compound-nucleus theories.     

Few-photon multiple ionization of ne and ar by strong free-electron-laser pulses

Few-photon multiple ionization of Ne and Ar atoms by strong vacuum ultraviolet laser pulses from the free-electron laser at Hamburg was investigated differentially with the Heidelberg reaction microscope. The light-intensity dependence of Ne2+ production reveals the dominance of nonsequential two-photon double ionization at intensities of I<6x10(12) W/cm2 and significant contributions of three-photon ionization as I increases. Ne2+ recoil-ion-momentum distributions suggest that two electrons absorbing "instantaneously" two photons are ejected most likely into opposite hemispheres with similar energies.     

Special features of electron beam-excited XeCl-laser generation

The results of experimental investigations on generation in Ar(Ne): Xe: CCl₄(HCl) mixtures at excitation by an electron beam are given. It is shown that the use of CCl₄ and HCl with an Ar buffer gas gives equal radiative energies and efficiencies and ā change of Ne for Ar causes a change in generation spectrum. The special features of XeCl-laser generation are discussed.     

Formation and migration properties of the rare gases He,Ne, Ar,Kr, and Xe in nickel

The energies of formation and migration of various rare gas-point defect complexes in an f.c.c. nickel lattice have been calculated for He, Ne, Ar, Kr, and Xe. Formation energies of rare gas atoms at interstitial sites are compared with those in substitutional sites. Binding energies are presented for self-interstitials and vacancies trapped to the various rare gas substitutionals. We also present migration energies and migration paths for various rare gas interstitials and substitutionals with and without trapped vacancies and self-interstitials. The migration energies are compared with the breakup energies for the corresponding complexes. We find that divacancy-rare gas complexes are rather stable and will migrate at relatively low energies compared to other substitutional rare gas migration processes.     

Fine structure in theα decay of192Po

The production of energetic π^? at 0° has been measured in Ne+NaF and Ni+Ni collisions with incident energies between 1.3 and 2AGeV. In Ne+NaF collisions the investigation was extended to extreme subthreshold processes with lab momenta up to 4.5 GeV/c. In both systems at all incident energies the π^? production cross sections deviate in a systematic way from thermal distributions.     

Global features of intermediate mass fragment cross sections in Ne induced interactions

Inclusive cross sections of intermediate mass fragments (6Z16) have been measured in ²⁰Ne induced reactions on silver and gold targets at 20, 30, 40, 50 and 60 MeV/u incident energies. Whereas the production yields remain approximately constant for the Ne+Ag system, they increase by a factor of two for the Ne+Au system over the same bombarding energy range. These results are discussed in the framework of two fragmentation models.     

Excitation spectra of the intrinsic luminescence of solid neon

The excitation spectra are measured for the atomic and the hot molecular self-trapped exciton (STE) luminescence in solid Ne. The atomic STE component is enhanced in comparison with the molecular STE at 17 and 19 eV of excitation energies, which are located at the low energy side of the bulk exciton transitions. On the other hand, the branching ratio into the atomic and the hot molecular STE's is almost constant at the other excitation energies.     

Self-trapped exciton bubble size growth in solid neon

A pseudopotential method is suggested for the calculation of the lattice perturbation on the absorption spectra of excited Ne atoms. The calculated shifts of the transition energies are very close to the experimental values. Different models are proposed in order to explain the formation process of a microcavity around the excited Ne atom.     

Non-Hermitian electronic theory and applications to clusters

Electronically excited cations, generated by inner-valence ionization of small molecules, relax in general by dissociation and photon emission. Autoionization is forbidden for energetic reasons. The situation changes fundamentally in an inner-valence ionized cluster, which releases its excess energy by emitting an electron. This novel process, referred to as Intermolecular Coulombic Decay, is characterized by an efficient energy transfer between monomers in the cluster. The decay is ultrafast, taking place on a femtosecond time scale. Theoretical tools are developed to predict the properties, in particular lifetimes, of molecular systems undergoing electronic decay. These methods are applied to study the relaxation of inner-valence holes in clusters. In order to enable a treatment of the scattering and the many-particle problem with standard electronic correlation methods for bound states, a complex absorbing potential is added to the Hamiltonian. Conceptual as well as practical aspects of this procedure are discussed in detail.     

On the He(I) and Ne(I) photoelectron spectra of OCS

The He(I) (58.43 nm) and Ne(I) (73.59–74.37 nm) photoelectron spectra of carbonyl sulphide have been reinvestigated at an improved resolution and a high signal-to-noise ratio; deconvolution of the data was carried out to aid interpretation of the spectra. Improved values are deduced for the vibrational wavenumbers and the ionization energies. The spin—orbit components of the Ã²Π II level are well resolved and a value of 135 cm^?1 (17 ± 5 meV) is proposed for the splitting. Perturbations in the relative intensities are observed in the Ne(I) spectrum; they suggest that the autoionizing Rydberg state located around 73.7 nm is excited by the 73.59 nm Ne(I) line and contributes to populate, with different probabilities, the ionic levels of lower energy, and particularly the X?²Π state.     

Oscillations due to two-electron exchange during He-Ne collisions

Ne (-)(1s(2)2s(2)2p(5)3s(2)) and He (-)(1s2s(2)) autodetachment peaks in electron spectra arising from He-Ne collisions at energies ranging from 350 eV to 6 keV have been measured. The areas of these two peaks are found to oscillate approximately in antiphase, with a constant wavelength, on a (velocity)(-1) scale. It is shown that this behavior can be explained by the "quasiresonance" situation for the separating particles in the channels Ne (-)-He (+) and He (-)-Ne (+). This explanation implies that the oscillations can be understood as being due to the simultaneous "hopping" of two electrons.