S. Voss

Multiorbital Tunneling Ionization of the CO Molecule

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.

Interatomic Coulombic Decay following Photoionization of the Helium Dimer: Observation of Vibrational Structure

Using synchrotron radiation we simultaneously ionize and excite one helium atom of a helium dimer (He2) in a shakeup process. The populated states of the dimer ion [i.e., He(*+)(n = 2, 3) - He] are found to deexcite via interatomic Coulombic decay. This leads to the emission of a second electron from the neutral site and a subsequent Coulomb explosion. In this Letter we present a measurement of the momenta of fragments that are created during this reaction. The electron energy distribution and the kinetic energy release of the two He+ ions show pronounced oscillations which we attribute to the structure of the vibrational wave function of the dimer ion.

Post ionization alignment of the fragmentation of molecules in an ultrashort intense laser field

We studied the angular distributions of the fragmented ions of diatomic molecules in an intense linearly polarized short laser pulse. In addition to the well-known dynamic alignment of the neutral molecules before ionization, we identified a more important post ionization alignment effect of the molecular ions. The latter is modelled quantum mechanically as resulting from the breakup of a rotating linear rotor. We showed that only for very short pulses are the two alignment mechanisms not important. In this case the angular distributions of the fragmented ions mimic the shape of the electronic density of the outermost molecular orbital.

Probing the tunnelling site of electrons in strong field enhanced ionization of molecules

Molecules show a much increased multiple ionization rate in a strong laser field as compared with atoms of similar ionization energy. A widely accepted model attributes this to the action of the joint fields of the adjacent ionic core and the laser on its neighbour inside the same molecule. The underlying physical picture for the enhanced ionization is that it is the up-field atom that gets ionized. However, this is still debated and remains unproven. Here we report an experimental verification of this long-standing prediction. This is accomplished by probing the two-site double ionization of ArXe, where the instantaneous field direction at the moment of electron release and the emission direction of the correlated ionizing centre are measured by detecting the recoil sum- and relative-momenta of the fragment ions. Our results unambiguously prove the intuitive picture of the enhanced multielectron dissociative ionization of molecules and clarify a long-standing controversy.

High resolution kinetic energy release spectra and angular distributions from double ionization of nitrogen and oxygen by short laser pulses

We have used momentum imaging techniques to measure in high resolution the kinetic energy release spectra and angular distributions of coincident O + and N + ion pairs produced by short laser pulses (8–35 fs) on targets of N2 and O2 at peak intensities between 1 and 12 × 10 14 Wc m −2 . We record the full momentum vectors of both members of each pair and achieve a kinetic energy release resolution of less than 0.3 eV. We find that the process proceeds through well-defined electronic states of the excited molecular dications. Using linear and circularly polarized light, we identify two mechanisms for the production of these states, rescattering and sequential ionization. By using 8 fs pulses, we observe that the internuclear distance can be frozen during the pulse. For low intensities and 8 fs pulses, emission from N2 is strongly directed along the polarization vector, while that for O2 is not, a result we interpret as being due to the different symmetries of the outer orbitals of these molecules. For high intensities and longer pulses, the distributions increasingly fold towards the polarization vector, ultimately peaking at zero degrees for both molecules. For oxygen, a local peaking for molecules aligned at right angles to the polarization vector is seen. A discussion and interpretation of the results are presented. (Some figures in this article are in colour only in the electronic version)

Nonadiabatic alignment of van der Waals-force-bound argon dimers by femtosecond laser pulses

We demonstrated that the weak van der Waals–force-bound argon dimer can be nonadiabatically aligned by nonresonant femtosecond laser pulses, showing periodic alignment and anti-alignment revivals after the extinction of the laser pulse. Based on the measured nonadiabatic alignment trace, the rotational constant of the argon dimer ground state is determined to be B0 = 0.05756 ± 0.00004 cm −1 . Noticeable alignment dependence of frustrated tunneling ionization and bond-softening induced dissociation of the argon dimer are observed.

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.