T. Osipov

Complete photo-fragmentation of the deuterium molecule

All properties of molecules—from binding and excitation energies to their geometry—are determined by the highly correlated initial-state wavefunction of the electrons and nuclei. Details of these correlations can be revealed by studying the break-up of these systems into their constituents. The fragmentation might be initiated by the absorption of a single photon, by collision with a charged particle or by exposure to a strong laser pulse: if the interaction causing the excitation is sufficiently understood, the fragmentation process can then be used as a tool to investigate the bound initial state. The interaction and resulting fragment motions therefore pose formidable challenges to quantum theory. Here we report the coincident measurement of the momenta of both nuclei and both electrons from the single-photon-induced fragmentation of the deuterium molecule. The results reveal that the correlated motion of the electrons is strongly dependent on the inter-nuclear separation in the molecular ground state at the instant of photon absorption.

K-shell photoionization of CO and N2: is there a link between the photoelectron angular distribution and the molecular decay dynamics?

We have used COLTRIMS to measure the angular distribution of electrons released from the K-shell of N2 and the carbon K-shell of CO by absorption of one linear polarized photon. For each ionization event which leads to two charged fragments we determine the angle of the photoelectron with respect to the fragment ion momenta. In addition we determine the charge state and energy of the molecular fragments. We find a breakdown of the axial recoil approximation for CO for kinetic energy releases below 10.2 eV, whereas for N2 that approximation is found to be valid for all fragment energies. Furthermore, the photoelectron emission spectrum for N2 is found to be the same for the molecular breakup channels producing N + N + and N + N ++ . (Some figures in this article are in colour only in the electronic version)

Momentum-imaging investigations of the dissociation of D2+ and the isomerization of acetylene to vinylidene by intense short laser pulses

We present momentum images of the ionic products from the ionization of D2 and C2H2 by short laser pulses. For D2, we use a pump–probe approach to investigate the dependence of the enhanced ionization on the internuclear distance. Evidence for two (not well separated) regions of enhancement is found near internuclear distances of 6 and 10 au. In the case of acetylene, we report clear evidence for the production of both acetylene and vinylidene dications with kinetic energy releases similar to those reported earlier by core electron removal. We also find very different angular distributions for the fragments in the two channels, consistent with a finite time for the isomerization.

Energy sharing and asymmetry parameters for photo double ionization of helium 100 eV above threshold in single-particle and Jacobi coordinates

We present a joint experimental and theoretical study of the double differential cross section for the double ionization of helium by absorption of one 179 eV linear polarized photon (100 eV above threshold). We show the energy sharing and the asymmetry parameters in both single-particle coordinates and in Jacobi coordinates. An asymmetric sharing of the electron excess energy and a breakup of the electron pair preferentially parallel to the polarization axis is found. This marks a deviation from the propensity rule favouring perpendicular relative electron motion which has been observed to hold at energies closer to the double-ionization threshold.

Photo double ionization of helium 100 eV and 450 eV above threshold: III. Gerade and ungerade amplitudes and their relative phases

We present a joint experimental and theoretical study of the gerade and ungerade amplitudes of the photo double ionization of helium at excess energies of 100 eV and 450 eV above the threshold. We describe a method of extracting the amplitudes from a COLTRIMS data set. The experimental results are well reproduced by convergent close-coupling (CCC) calculations. The fully differential cross section data underlying this study can be found in our companion papers immediately preceding this one.

Photo double ionization of helium 100 eV and 450 eV above threshold: I. Linearly polarized light

We present a joint experimental and theoretical study for the fully differential cross section of the photo double ionization (PDI) of helium with linearly polarized light at the excess energies Eexc = 100 eV and 450 eV above the threshold. The fully differential cross section is obtained by measuring the three-dimensional momentum vectors of one electron and the He 2+ ion in coincidence using the COLTRIMS method. We give an overview of the momentum distribution of the three-body continuum 100 eV above the threshold. We show angular distributions for both electrons for various energy sharings at Eexc = 100 eV and 450 eV. The experimental results are well reproduced by a set of convergent close-coupling (CCC) calculations.

Photon-ion collisions and molecular clocks

The timing of molecular rearrangements can be followed in the time domain on a femtosecond scale by using momentum imaging techniques. Three examples are discussed in this paper: first, the diffraction of electrons ejected from the K-shell of one of the atomic constituents of the molecule takes a ‘picture’ of the molecule, and the correlation between the momentum vector of the photoelectron and the subsequent fragmentation pattern is used to estimate the time delay which accompanies the latter process. Second, the kinetic energy release of proton pairs from the double ionization of hydrogen by fast laser pulses is timed using the optical cycle as a clock. The mechanisms of rescattering, sequential and enhanced ionization are clearly identified in the momentum spectra. Third, the operation of rescattering double ionization in the case of nitrogen and oxygen molecules is discussed.

Photo- and charged-particle-ionization of He and D2 studied with COLTRIMS

The COLTRIMS (COLd Target Recoil Ion Momentum Spectroscopy) approach to final-state momentum imaging is now being widely used in at least a dozen accelerator and synchrotron-radiation laboratories in the world and its use is growing rapidly. The technique combines fast imaging detectors with a supersonically cooled gas target to allow the charged particles from a collision, including both recoil ions and electrons, to be collected with extremely high efficiency and with fully measured vector momenta. It allows the investigation of correlations between ejected momentum fragments and in some cases the identification of collective modes of disintegration. When molecular targets are used, it allows the a posteriori determination of the alignment of the molecule at the time of the collision. We will discuss the use of this approach to study the single and double ionization of He and D2 by the impact of photons and of charged particles over a wide range of velocities.