We report on nonsequential double ionization of Ar by a laser pulse consisting of two counterrotating circularly polarized fields (390 and 780 nm). The double-ionization probability depends strongly ...on the relative intensity of the two fields and shows a kneelike structure as a function of intensity. We conclude that double ionization is driven by a beam of nearly monoenergetic recolliding electrons, which can be controlled in intensity and energy by the field parameters. The electron momentum distributions show the recolliding electron as well as a second electron which escapes from an intermediate excited state of Ar^{+}.
When a strong laser pulse induces the ionization of an atom, momentum conservation dictates that the absorbed photons transfer their momentum to the electron and its parent ion. The sharing of the ...photon momentum between the two particles and its underlying mechanism in strong-field ionization, occurring when the bound electron tunnels through the barrier created by the superposition of the atomic potential and the electric laser field, are still debated in theory1–4 after 30 years of research. Corresponding experiments are very challenging due to the extremely small photon momentum and their precision has been too limited, so far, to ultimately resolve this debate5–8. By utilizing an experimental approach relying on two counter-propagating laser pulses, we present a detailed study of the effects of the photon momentum in strong-field ionization. The high precision of the method and the intrinsically known zero momentum allow us to unambiguously demonstrate the action of the light’s magnetic field on the electron while it is under the tunnel barrier, which has only been theoretically predicted so far1–3,9, thereby disproving opposing predictions5,10,11. Our results deepen the understanding of, for example, molecular imaging12,13 and time-resolved photoelectron holography14.
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.
At the transition from the gas to the liquid phase of water, a wealth of new phenomena emerge, which are absent for isolated H2O molecules. Many of those are important for the existence of life, for ...astrophysics and atmospheric science. In particular, the response to electronic excitation changes completely as more degrees of freedom become available. Here we report the direct observation of an ultrafast transfer of energy across the hydrogen bridge in (H2O)2 (a so-called water dimer). This intermolecular coulombic decay leads to an ejection of a low-energy electron from the molecular neighbour of the initially excited molecule. We observe that this decay is faster than the proton transfer that is usually a prominent pathway in the case of electronic excitation of small water clusters and leads to dissociation of the water dimer into two H2O+ ions. As electrons of low energy (∼0.7-20 eV) have recently been found to efficiently break-up DNA constituents, the observed decay channel might contribute as a source of electrons that can cause radiation damage in biological matter.
During the past 15 years a novel decay mechanism of excited atoms has been discovered and investigated. This so-called interatomic Coulombic decay (ICD) involves the chemical environment of the ...electronically excited atom: the excitation energy is transferred (in many cases over long distances) to a neighbor of the initially excited particle usually ionizing that neighbor. It turned out that ICD is a very common decay route in nature as it occurs across van der Waals and hydrogen bonds. The time evolution of ICD is predicted to be highly complex, as its efficiency strongly depends on the distance of the atoms involved and this distance typically changes during the decay. Here we present the first direct measurement of the temporal evolution of ICD using a novel experimental approach.
We investigate the temporal evolution of molecular frame angular distributions of Auger electrons emitted during ultrafast dissociation of HCl following a resonant single-photon excitation. The ...electron emission pattern changes its shape from that of a molecular σ orbital to that of an atomic p state as the system evolves from a molecule into two separated atoms.
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.
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.
We report on the observation of discrete structures in the electron energy distribution for strong field double ionization of argon at 394 nm. The experimental conditions were chosen in order to ...ensure a nonsequential ejection of both electrons with an intermediate rescattering step. We have found discrete above-threshold ionization like peaks in the sum energy of both electrons, as predicted by all quantum mechanical calculations. More surprisingly, however, is the observation of two above-threshold ionization combs in the energy distribution of the individual electrons.
Electron motion in chemical bonds occurs on an attosecond timescale. This ultrafast motion can be driven by strong laser fields. Ultrashort asymmetric laser pulses are known to direct electrons to a ...certain direction. But do symmetric laser pulses destroy symmetry in breaking chemical bonds? Here we answer this question in the affirmative by employing a two-particle coincidence technique to investigate the ionization and fragmentation of H₂ by a long circularly polarized multicycle femtosecond laser pulse. Angular streaking and the coincidence detection of electrons and ions are employed to recover the phase of the electric field, at the instant of ionization and in the molecular frame, revealing a phase-dependent anisotropy in the angular distribution of H⁺ fragments. Our results show that electron localization and asymmetrical breaking of molecular bonds are ubiquitous, even in symmetric laser pulses. The technique we describe is robust and provides a powerful tool for ultrafast science.
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