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Absolute Images Molecules are held together by a balance of charge between negative electrons and positive nuclei. When multiple electrons are expelled by laser irradiation, the remaining, mutually repulsive nuclei fly apart in a Coulomb explosion. Instead of traditional x-ray diffraction methods that require crystalline samples, Pitzer et al. (p. 1096 ) show that by tracking the fragment trajectories from laser-induced Coulomb explosions of relatively simple gas phase molecules, they can determine the absolute stereochemical configuration of enantiomers (mirror-image isomers).

Controlling the interactions between atoms with external fields opened up new branches in physics ranging from strongly correlated atomic systems to ideal Bose1 and Fermi2 gases and Efimov physics3,4. Such control usually prepares samples that are stationary or evolve adiabatically in time. In contrast, in molecular physics, external ultrashort laser fields are used to create anisotropic potentials that launch ultrafast rotational wave packets and align molecules in free space5. Here we combine these two regimes of ultrafast times and low energies. We apply a short laser pulse to the helium dimer, a weakly bound and highly delocalized single bound state quantum system. The laser field locally tunes the interaction between two helium atoms, imparting an angular momentum of 2ℏ and evoking an initially confined dissociative wave packet. We record a video of the density and phase of this wave packet as it propagates from small to large internuclear distances. At large internuclear distances, where the interaction between atoms is negligible, the wave packet is essentially free. This work paves the way for future tomography of wave-packet dynamics and provides the technique for studying exotic and otherwise hardly accessible quantum systems, such as halo and Efimov states. Ultrashort laser fields applied to a helium dimer are able to tune the interactions between two helium atoms. A video of the dimer’s response to this localized disturbance shows the effect of dissociation and alignment of the wave packets.

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. Experiments with two counter-propagating laser beams report the observation that the photon momentum is shared between the electron and parent ion in strong-field ionization, which results from the photon’s magnetic field acting on the electron.

Strong-field ionization of atoms by circularly polarized femtosecond laser pulses produces a donut-shaped electron momentum distribution. Within the dipole approximation this distribution is symmetric with respect to the polarization plane. The magnetic component of the light field is known to shift this distribution forward. Here, we show that this magnetic non-dipole effect is not the only non-dipole effect in strong-field ionization. We find that an electric non-dipole effect arises that is due to the position dependence of the electric field and which can be understood in analogy to the Doppler effect. This electric non-dipole effect manifests as an increase of the radius of the donut-shaped photoelectron momentum distribution for forward-directed momenta and as a decrease of this radius for backwards-directed electrons. We present experimental data showing this fingerprint of the electric non-dipole effect and compare our findings with a classical model and quantum calculations., 6 pages, 3 figures

Physical review letters 123(24), 243201 (2019). doi:10.1103/PhysRevLett.123.243201, We investigate angular emission distributions of the 1s photoelectrons of N2 ionized by linearlypolarized synchrotron radiation at hν ¼ 40 keV. As expected, nondipole contributions cause a very strongforward-backward asymmetry in the measured emission distributions. In addition, we observe anunexpected asymmetry with respect to the polarization direction, which depends on the direction ofthe molecular fragmentation. In particular, photoelectrons are predominantly emitted in the direction of theforward nitrogen atom. This observation cannot be explained via asymmetries introduced by the initialbound and final continuum electronic states of the oriented molecule. The present simulations assign thisasymmetry to a novel nontrivial effect of the recoil imposed to the nuclei by the fast photoelectrons andhigh-energy photons, which results in a propensity for the ions to break up along the axis of the recoilmomentum. The results are of particular importance for the interpretation of future experiments at x-rayfree electron lasers operating in the few tens of keV regime, where such nondipole and recoil effects will beessential., Published by APS, College Park, Md.

Physical review research 2(3), 1-7 (2020). doi:10.1103/PhysRevResearch.2.033080, We report on kinematically complete measurements and ab initio nonperturbative calculations of double ionization of He and H2 by a single 800 eV circularly polarized photon. We confirm the quasifree mechanism of photoionization for H2 and show how it originates from the two-electron cusp in the ground state of a two-electron target. Our approach establishes a method for mapping electrons relative to each other and provides valuable insight into photoionization beyond the electric-dipole approximation., Published by APS, College Park, MD

Physical review letters 124(23), 233201 (2020). doi:10.1103/PhysRevLett.124.233201, We experimentally investigate the effects of the linear photon momentum on the momentum distributions of photoions and photoelectrons generated in one-photon ionization in an energy range of 300 eV≤E$_\gamma$≤40 keV. Our results show that for each ionization event the photon momentum is imparted onto the photoion, which is essentially the system’s center of mass. Nevertheless, the mean value of the ion momentum distribution along the light propagation direction is backward-directed by −3/5 times the photon momentum. These results experimentally confirm a 90-year-old prediction., Published by APS, College Park, Md.

We experimentally and theoretically show that the electron energy spectra strongly depend on the relative helicity in highly intense, circularly polarized two-color laser fields which is an unexpected finding. The employed counter-rotating two-color (CRTC) fields and the co-rotating two-color (CoRTC) fields are both a superposition of circularly polarized laser pulses at a central wavelength of 390 nm and 780 nm (intensitiy ratio $I_{390}/I_{780}\approx 250$). For the CRTC field, the measured electron energy spectrum is dominated by peaks that are spaced by 3.18 eV (corresponds to the photon energy of light at a wavelength of 390 nm). For the CoRTC field, we observe additional energy peaks (sidebands). Using our semi-classical, trajectory-based models, we conclude that the sideband intensity is modulated by a sub-cycle interference, which sensitively depends on the relative helicity in circularly polarized two-color fields., 7 pages, 4 figures

We report on the unambiguous observation of the subcycle ionization bursts in sequential strong-field double ionization of H_{2} and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase, in combination with multiparticle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state-specific Coulomb distortions on emitted electrons in polyatomic molecules.

Science 370(6514), 339 - 341 (2020). doi:10.1126/science.abb9318, Photoionization is one of the fundamental light-matter interaction processes in which the absorption of a photon launches the escape of an electron. The time scale of this process poses many open questions. Experiments have found time delays in the attosecond (10$^{-18}$ seconds) domain between electron ejection from different orbitals, from different electronic bands, or in different directions. Here, we demonstrate that, across a molecular orbital, the electron is not launched at the same time. Rather, the birth time depends on the travel time of the photon across the molecule, which is 247 zeptoseconds (1 zeptosecond = 10$^{-21}$ seconds) for the average bond length of molecular hydrogen. Using an electron interferometric technique, we resolve this birth time delay between electron emission from the two centers of the hydrogen molecule., Published by Moses King, Cambridge, Mass.

Journal of physics / B 53(19), 1-6 (2020). doi:10.1088/1361-6455/aba3d3 special issue: "Special issue on Frontiers of AMO Science with FELs and Synchrotron Radiation", The angular distribution of O 1s photoelectrons emitted from uniaxially oriented methanol is studied experimentally and theoretically. We employed circularly polarized photons of an energy of hν = 550 eV for our investigations. We measured the three-dimensional photoelectron angular distributions of methanol, with the CH3–OH axis oriented in the polarization plane, by means of cold target recoil ion momentum spectroscopy. The experimental results are interpreted by single active electron calculations performed with the single center method. A comparative theoretical study of the respective molecular-frame angular distributions of O 1s photoelectrons of CO, performed for the same photoelectron kinetic energy and for a set of different internuclear distances, allows for disentangling the role of internuclear distance and the hydrogen atoms of methanol as compared to carbon monoxide., Published by IOP Publ., Bristol

Physical review letters 124(4), 043201 (2020). doi:10.1103/PhysRevLett.124.043201, We theoretically and experimentally investigate the photon momentum transfer in single-photon double ionization of helium at various large photon energies. We find that the forward shifts of the momenta along the light propagation of the two photoelectrons are roughly proportional to their fraction of the excess energy. The mean value of the forward momentum is about $8/5$ of the electron energy divided by the speed of light. This holds for fast and slow electrons despite the fact that the energy sharing is highly asymmetric and the slow electron is known to be ejected by secondary processes of shake off and knockout rather than directly taking its energy from the photon. The biggest deviations from this rule are found for the region of equal energy sharing where the quasifree mechanism dominates double ionization., Published by APS, College Park, Md.

Synopsis The spectator resonant interatomic Coulombic decay (SRICD) following the 2s →5p excitation of Ne dimers has been examined experimentally and theoretically. The molecular frame angular distributions (MFADs) of the SRICD electrons depend strongly on the direction of the polarization vector of the exciting photon with respect to the molecular axis. We demonstrate that this effect is caused by the scattering of the low-energy SRICD electron on the density of the spectator electron.

Compton scattering is one of the fundamental interaction processes of light with matter. When discovered1, it was described as a billiard-type collision of a photon ‘kicking’ a quasi-free electron. With decreasing photon energy, the maximum possible momentum transfer becomes so small that the corresponding energy falls below the binding energy of the electron. In this regime, ionization by Compton scattering becomes an intriguing quantum phenomenon. Here, we report on a kinematically complete experiment studying Compton scattering off helium atoms in that regime. We determine the momentum correlations of the electron, the recoiling ion and the scattered photon in a coincidence experiment based on cold target recoil ion momentum spectroscopy, finding that electrons are not only emitted in the direction of the momentum transfer, but that there is a second peak of ejection to the backward direction. This finding links Compton scattering to processes such as ionization by ultrashort optical pulses2, electron impact ionization3,4, ion impact ionization5,6 and neutron scattering7, where similar momentum patterns occur. Compton scattering experiments off helium atoms for photon energies close to the ionization threshold reveal that electrons are not only emitted in the direction of the momentum transfer but also backwards.

We report observations of the interatomic Coulombic decay (ICD) and electron-transfer-mediated decay (ETMD) from the triply charged states in Ne2 and NeAr dimers. The ICD processes leading to fragmentation of Ne3+-Ne into Ne3+-Ne+ and Ne3+-Ar into Ne3+-Ar+, and ETMD processes leading to fragmentation of Ne3+-Ne into Ne2+-Ne2+ are unambiguously identified by electron–ion-ion coincidence spectroscopy in which the kinetic energy of the ICD or ETMD electron and the kinetic energy release between the two fragment ions are measured in coincidence.

In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned. Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ ( R ) of the decay is obtained from the measured kinetic energy release distribution of the ions employing a classical nuclear dynamics model.

Coulomb explosion of diiodomethane CH2I2 molecules irradiated by ultrashort and intense X-ray pulses from SACLA, the Japanese X-ray free electron laser facility, was investigated by multi-ion coincidence measurements and self-consistent charge density-functional-based tight-binding (SCC-DFTB) simulations. The diiodomethane molecule, containing two heavy-atom X-ray absorbing sites, exhibits a rather different charge generation and nuclear motion dynamics compared to iodomethane CH3I with only a single heavy atom, as studied earlier. We focus on charge creation and distribution in CH2I2 in comparison to CH3I. The release of kinetic energy into atomic ion fragments is also studied by comparing SCC-DFTB simulations with the experiment. Compared to earlier simulations, several key enhancements are made, such as the introduction of a bond axis recoil model, where vibrational energy generated during charge creation processes induces only bond stretching or shrinking. We also propose an analytical Coulomb energy partition model to extract the essential mechanism of Coulomb explosion of molecules from the computed and the experimentally measured kinetic energies of fragment atomic ions by partitioning each pair Coulomb interaction energy into two ions of the pair under the constraint of momentum conservation. Effective internuclear distances assigned to individual fragment ions at the critical moment of the Coulomb explosion are then estimated from the average kinetic energies of the ions. We demonstrate, with good agreement between the experiment and the SCC-DFTB simulation, how the more heavily charged iodine fragments and their interplay define the characteristic features of the Coulomb explosion of CH2I2. The present study also confirms earlier findings concerning the magnitude of bond elongation in the ultrashort X-ray pulse duration, showing that structural damage to all but C–H bonds does not develop to a noticeable degree in the pulse length of ∼10 fs.

We study the decay of a helium/neon dimer after ionization and simultaneous excitation of either the neon or the helium atom using Cold Target Recoil Ion Momentum Spectroscopy (COLTRIMS). We find that, depending on the decaying state, either direct Interatomic Coulombic Decay (ICD) (i.e. mediated by a virtual photon exchange), exchange ICD (mediated by electron exchange) or radiative charge transfer occurs. The corresponding channels are identified.

Proceedings of the National Academy of Sciences of the United States of America 113(51), 14651 – 14655 (2016). doi:10.1073/pnas.1610688113, Quantum tunneling is a ubiquitous phenomenon in nature and crucial for many technological applications. It allows quantum particles to reach regions in space which are energetically not accessible according to classical mechanics. In this “tunneling region,” the particle density is known to decay exponentially. This behavior is universal across all energy scales from nuclear physics to chemistry and solid state systems. Although typically only a small fraction of a particle wavefunction extends into the tunneling region, we present here an extreme quantum system: a gigantic molecule consisting of two helium atoms, with an 80% probability that its two nuclei will be found in this classical forbidden region. This circumstance allows us to directly image the exponentially decaying density of a tunneling particle, which we achieved for over two orders of magnitude. Imaging a tunneling particle shows one of the few features of our world that is truly universal: the probability to find one of the constituents of bound matter far away is never zero but decreases exponentially. The results were obtained by Coulomb explosion imaging using a free electron laser and furthermore yielded He2’s binding energy of 151.9 +-13.3 neV, which is in agreement with most recent calculations., Published by National Acad. of Sciences, Washington, DC

The increasing availability of X-ray free-electron lasers (XFELs) has catalyzed the development of single-object structural determination and of structural dynamics tracking in real-time. Disentangling the molecular-level reactions triggered by the interaction with an XFEL pulse is a fundamental step towards developing such applications. Here we report real-time observations of XFEL-induced electronic decay via short-lived transient electronic states in the diiodomethane molecule, using a femtosecond near-infrared probe laser. We determine the lifetimes of the transient states populated during the XFEL-induced Auger cascades and find that multiply charged iodine ions are issued from short-lived (∼20 fs) transient states, whereas the singly charged ones originate from significantly longer-lived states (∼100 fs). We identify the mechanisms behind these different time scales: contrary to the short-lived transient states which relax by molecular Auger decay, the long-lived ones decay by an interatomic Coulombic decay between two iodine atoms, during the molecular fragmentation., X線照射で始まる超高速反応の観測に成功 --レントゲンによるX線の発見から120年で初--. 京都大学プレスリリース. 2019-05-28.

We demonstrate two-dimensional control over the chargelocalization in H2 dissociation using elliptically polarized laser pulses. The influences of the CEP and the laser phase at the instant of ionization are investigated.

We investigate $K$-shell ionization of ${\mathrm{N}}_{2}$ at 40 keV photon energy. Using a cold target recoil ion momentum spectroscopy reaction microscope, we determine the vector momenta of the photoelectron, the Auger electron, and both ${\mathrm{N}}^{+}$ fragments. These fully differential data show that the dissociation process of the ${\mathrm{N}}_{2}^{2+}$ ion is significantly modified not only by the recoil momentum of the photoelectron but also by the photon momentum and the momentum of the emitted Auger electron. We find that the recoil energy introduced by the photon and the photoelectron momentum is partitioned with a ratio of approximately $30\ensuremath{\mathbin:}70$ between the Auger electron and fragment ion kinetic energies, respectively. We also observe that the photon momentum induces an additional rotation of the molecular ion.

Physical review / A covering atomic, molecular, and optical physics and quantum information 100(2), 022707 (2019). doi:10.1103/PhysRevA.100.022707, We report on the experimental observation of interatomic Coulombic decay (ICD) in pure 4He nanoclustersof mean sizes between N ∼ 5000 and 30 000 and the subsequent scattering of energetic He+ fragments insidethe neutral cluster by using cold target recoil ion momentum spectroscopy. ICD is induced in He clusters byusing vacuum ultraviolet light of hν = 67 eV from the BESSY II synchrotron. The electronic decay createstwo neighboring ions in the cluster at a well-defined distance. The measured fragment energies and angularcorrelations show that a main energy loss mechanism of these ions inside the cluster is a single hard binarycollision with one atom of the cluster., Published by Inst., Woodbury, NY

Physical review letters 123(4), 043202 (2019). doi:10.1103/PhysRevLett.123.043202, It is commonly accepted that the magnitude of a photoelectron circular dichroism (PECD) is governed by the ability of an outgoing photoelectron wave packet to probe the chiral asymmetry of a molecule. To be able to accumulate this characteristic asymmetry while escaping the chiral ion, photoelectrons need to have relatively small kinetic energies of up to a few tens of electron volts. Here, we demonstrate a substantial PECD for very fast photoelectrons above 500 eV kinetic energy released from methyloxirane by a participator resonant Auger decay of its lowermost O $1s$ excitation. This effect emerges as a result of the Fano interference between the direct and resonant photoionization pathways, notwithstanding that their individual effects are negligibly small. The resulting dichroic parameter has an anomalous dispersion: It changes its sign across the resonance, which can be considered as an analogue of the Cotton effect in the x-ray regime., Published by APS, College Park, Md.

We introduce and employ the molecular attoclock method. This allows us to simultaneously trace the nuclear and electron dynamics during H2 fragmentation, and to CEP-control the two-electron emission dynamics on sub-cycle time scales., High Intensity Lasers and High Field Phenomena, 26–28 March, 2018, Strasbourg, France

Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference., The wave nature of light and particles is of interest to the fundamental quantum mechanics. Here the authors show the double-slit interference effect in the strong-field ionization of neon dimers by employing COLTRIMS method to record the momentum distribution of the photoelectrons in the molecular frame

We introduce a concise methodology to detect the parity of atomic and molecular orbitals based on photoelectron holography, which is more general than the existing schemes. It fully accounts for the Coulomb distortions of electron trajectories, does not require sculpted fields to retrieve phase information and, in principle, is applicable to a broad range of electron momenta. By comparatively measuring the differential photoelectron spectra from strong-field ionization of ${\mathrm{N}}_{2}$ molecules and their companion atoms of Ar, some photoelectron holography patterns are found to be dephased for both targets. This is well reproduced by the full-dimensional time-dependent Schr\"odinger equation and the Coulomb quantum-orbit strong-field approximation (CQSFA) simulation. Using the CQSFA, we trace back our observations to different parities of the $3p$ orbital of Ar and the highest-occupied molecular orbital of ${\mathrm{N}}_{2}$ via interfering Coulomb-distorted quantum orbits carrying different initial phases. This method could in principle be used to extract bound-state phases from any holographic structure, with a wide range of potential applications in recollision physics and spectroscopy.

Synopsis The installation of a reaction microscope (COLTRIMS [1]) in the electrostatic Frankfurt Low Energy Storage Ring (FLSR) [2] has been completed. A first experiment, exploring the KER for dissociative electron transfer to HeH+ ions at 20 keV from a cold supersonic He gas target have been carried. Even at the moderate vacuum of 10−8 mbar a change of the KER and the Q value distribution due to cooling of the molecular ions during the storage time can be observed. In this contribution the final experiment, performed after heating the ring will be discussed.

Physical review letters 121(24), 243002 (2018). doi:10.1103/PhysRevLett.121.243002, We suggest that low-energy electrons, released by resonant decay processes, experience substantial scattering on the electron density of excited electrons, which remain a spectator during the decay. As a result, the angular emission distribution is altered significantly. This effect is expected to be a common feature of low-energy secondary electron emission. In this Letter, we exemplify our idea by examining the spectator resonant interatomic Coulombic decay of Ne dimers. Our theoretical predictions are confirmed by a corresponding coincidence experiment., Published by APS, College Park, Md.

We report on the non-adiabatic offset of the initial electron momentum distribution in the plane of polarization upon single ionization of argon by strong field tunneling and show how to experimentally control the degree of non-adiabaticity. Two-color counter- and co-rotating fields (390 and 780 nm) are compared to show that the non-adiabatic offset strongly depends on the temporal evolution of the laser electric field. We introduce a simple method for the direct access to the non-adiabatic offset using two-color counter- and co-rotating fields. Further, for a single-color circularly polarized field at 780 nm we show that the radius of the experimentally observed donut-like distribution increases for increasing momentum in the light propagation direction. Our observed initial momentum offsets are well reproduced by the strong-field approximation (SFA). A mechanistic picture is introduced that links the measured non-adiabatic offset to the magnetic quantum number of virtually populated intermediate states., Comment: 6 pages, 4 figures

We report on a kinematically complete experiment on strong field double ionization of helium using laser pulses with a wavelength of 394\,nm and intensities of $3.5-5.7\times10^{14}\,W/cm^2$. Our experiment reaches the most complete level of detail which previously has only been reached for single photon double ionization. We give an overview over the observables on many levels of integration, starting from the ratio of double to single ionization, the individual electron and ion momentum distributions over joint momentum and energy distributions to fully differential cross sections showing the correlated angular momentum distributions. Within the studied intensity range the ratio of double to single ionization changes from $2\times 10^{-4}$ to $1.5\times 10^{-3}$. We find the momentum distributions of the $\rm{He}^{2+}$ ions and the correlated two electron momentum distributions to vary substantially. Only at the highest intensity both electrons are emitted to the same direction while at the lowest intensity back-to-back emission dominates. The joint energy distribution of the electrons shows discrete structures from the energy quantization of the photon field which allows us to count the number of absorbed photons and thus access the parity of the final state. We find the energy of the individual electron to show a peak structure indicating a quantized sharing of the overall energy absorbed from the field. The joint angular momentum distributions of the two electrons show a highly directed emission of both electrons along the polarization axis as well as clear imprints of electron repulsion. They strongly change with the energy sharing between the electrons. The aspect of selection rules in double ionization which are also visible in the presented dataset has been subject to a preceding publication [1]., 10 pages, 13 figures, submitted to PRA

We report on a direct method to measure the interatomic potential energy curve of diatomic systems. A cold target recoil ion momentum spectroscopy reaction microscope was used to measure the squares of the vibrational wave functions of H_{2}, He_{2}, Ne_{2}, and Ar_{2}. The Schrodinger equation relates the curvature of the wave function to the potential V(R) and therefore offers a simple but elegant way to extract the shape of the potential.

X-ray free-electron lasers (XFELs) made available a new regime of x-ray intensities, revolutionizing the ultrafast structure determination and laying the foundations of the novel field of nonlinear x-ray optics. Although earlier studies revealed nanoplasma formation when an XFEL pulse interacts with any nanometer-scale matter, the formation process itself has never been decrypted and its timescale was unknown. Here we show that time-resolved ion yield measurements combined with a near-infrared laser probe reveal a surprisingly ultrafast population (∼ 12 fs), followed by a slower depopulation (∼ 250 fs) of highly excited states of atomic fragments generated in the process of XFEL-induced nanoplasma formation. Inelastic scattering of Auger electrons and interatomic Coulombic decay are suggested as the mechanisms populating and depopulating, respectively, these excited states. The observed response occurs within the typical x-ray pulse durations and affects x-ray scattering, thus providing key information on the foundations of x-ray imaging with XFELs., プラズマ誕生の瞬間を観測 --X線自由電子レーザー照射によるプラズマ生成機構を解明--. 京都大学プレスリリース. 2018-09-20.

Author(s): Martin, L; Bello, RY; Hogle, CW; Palacios, A; Tong, XM; Sanz-Vicario, JL; Jahnke, T; Schoffler, M; Dorner, R; Weber, T; Martin, F; Kapteyn, HC; Murnane, MM; Ranitovic, P | Abstract: Understanding electron-electron correlations in matter ranging from atoms to solids represents a grand challenge for both experiment and theory. These correlations occur on attosecond timescales and have only recently become experimentally accessible. In the case of highly excited systems, the task of understanding and probing correlated interactions is even greater. In this work, we combine state-of-the-art light sources and advanced detection techniques with ab initio calculations to unravel the role of electron-electron correlation in D2 photoionization by mapping the dissociation of a highly excited D2+ molecule. Correlations between the two electrons dictate the pathways along which the molecule dissociates and lead to a superposition of excited ionic states. Using 3D Coulomb explosion imaging and electron-ion coincidence techniques, we assess the relative contribution of competing parent ion states to the dissociation process for different orientations of the molecule with respect to the laser polarization, which is consistent with a shake-up ionization process. As a step toward observing coherent superposition experimentally, we map the relevant nuclear potentials using Coulomb explosion imaging and show theoretically that such an experiment could confirm this coherence via two-path interference.

We present a joint experimental and theoretical investigation of the correlated electron momentum spectra from strong-field double ionization of neon induced by elliptically polarized laser pulses. A significant asymmetry of the electron momentum distributions along the major polarization axis is reported. This asymmetry depends sensitively on the laser ellipticity. Using a three-dimensional semiclassical model, we attribute this asymmetry pattern to the ellipticity-dependent probability distributions of recollision time. Our work demonstrates that, by simply varying the ellipticity, the correlated electron emission can be two-dimensionally controlled and the recolliding electron trajectories can be steered on a subcycle time scale.

Resonant interatomic Coulombic decay (RICD) has been studied with HeNe dimers, where two decay channels are identified by bound HeNe${}^{+}$ states and low-energetic He+Ne${}^{+}$ fragments, and the state-resolved angular emission distributions of respective RICD electrons are examined in detail.

Quantum particles can penetrate potential barriers by tunneling (1). If that barrier is rotating, the tunneling process is modified (2,3). This is typical for electrons in atoms, molecules or solids exposed to strong circularly polarized laser pulses (4,5). Here we measure how the transmission probability through a rotating tunnel depends on the sign of the magnetic quantum number m of the electron and thus on the initial sense of rotation of its quantum phase. We further show that the electron keeps part of that rotary motion on its way through the tunnel by measuring m-dependent modification of the electron emission pattern. These findings are relevant for attosecond metrology as well as for interpretation of strong field electron emission from atoms and molecules (6-13) and directly demonstrates the creation of ring currents in bound states of ions with attosecond precision. In solids, this could open a way to inducing and controlling ring-current related topological phenomena (14)., 19 pages, 6 figures, Nature Physics accepted

The spin polarization of electrons from multiphoton ionization of Xe by 395 nm circularly polarized laser pulses at $6\ifmmode\times\else\texttimes\fi{}{10}^{13}\text{ }\text{ }\mathrm{W}/{\mathrm{cm}}^{2}$ has been measured. At this photon energy of 3.14 eV the above-threshold ionization peaks connected to ${\mathrm{Xe}}^{+}$ ions in the ground state ($J=3/2$, ionization potential ${I}_{p}=12.1\text{ }\text{ }\mathrm{eV}$) and the first excited state ($J=1/2$, ${I}_{p}=13.4\text{ }\text{ }\mathrm{eV}$) are clearly separated in the electron energy distribution. These two combs of above-threshold ionization peaks show opposite spin polarizations. The magnitude of the spin polarization is a factor of 2 higher for the $J=1/2$ than for the $J=3/2$ final ionic state. In turn, the data show that the ionization probability is strongly dependent on the sign of the magnetic quantum number.

We examine correlated electron and doubly charged ion momentum spectra from strong field double ionization of Neon employing intense elliptically polarized laser pulses. An ellipticity-dependent asymmetry of correlated electron and ion momentum distributions has been observed. Using a 3D semiclassical model, we demonstrate that our observations reflect the sub-cycle dynamics of the recollision process. Our work reveals a general physical picture for recollision-impact double ionization with elliptical polarization, and demonstrates the possibility of ultrafast control of the recollision dynamics., Comment: 6 pages, 5 figures

International audience; Almost ten years ago, energetic neutral hydrogen atoms were detected after a strong-field double ionization of H2. This process, called 'frustrated tunneling ionization', occurs when an ionized electron is recaptured after being driven back to its parent ion by the electric field of a femtosecond laser. In the present study we demonstrate that a related process naturally occurs in clusters without the need of an external field: we observe a charge hopping that occurs during a Coulomb explosion of a small helium cluster, which leads to an energetic neutral helium atom. This claim is supported by theoretical evidence. As an analog to 'frustrated tunneling ionization', we term this process 'frustrated Coulomb explosion'.

We experimentally achieve two-dimensional CEP-control of bond breaking in H2 dissociation with elliptically polarized pulses. The lab and molecular frame of reference proton ejection asymmetries are compared.

As a fundamental property of the electron, the spin plays a decisive role in the electronic structure of matter from solids to molecules and atoms, e.g. causing magnetism. Yet, despite its importance, the spin dynamics of electrons released during the interaction of atoms with strong ultrashort laser pulses has remained unexplored. Here we report on the experimental detection of electron spin polarization by strong-field ionization of Xenon atoms and support our results by theoretical analysis. We found up to 30% spin polarization changing its sign with electron energy. This work opens the new dimension of spin to strong-field physics. It paves the way to production of subfemtosecond spin polarized electron pulses with applications ranging from probing magnetic properties of matter at ultrafast time scales to testing chiral molecular systems with subfemtosecond temporal and sub-{\AA}ngstr\"om spatial resolution., Comment: 9 pages, 3 figures

We report on the observation of phase space modulations in the correlated electron emission after strong field double ionization of helium using laser pulses with a wavelength of 394~nm and an intensity of $3\cdot10^{14}$W/cm$^2$. Those modulations are identified as direct results of quantum mechanical selection rules predicted by many theoretical calculations. They only occur for an odd number of absorbed photons. By that we attribute this effect to the parity of the continuum wave function., 5 pages, 3 figures, submitted to Phys. Rev. Lett

This article shows how the COLTRIMS (Cold Target Recoil Ion Momentum Spectroscopy) or the "reaction microscope" technique can be used to distinguish between enantiomers (stereoisomers) of simple chiral species on the level of individual molecules. In this approach, a gaseous molecular jet of the sample expands into a vacuum chamber and intersects with femtosecond (fs) laser pulses. The high intensity of the pulses leads to fast multiple ionization, igniting a so-called Coulomb Explosion that produces several cationic (positively charged) fragments. An electrostatic field guides these cations onto time- and position-sensitive detectors. Similar to a time-of-flight mass spectrometer, the arrival time of each ion yields information on its mass. As a surplus, the electrostatic field is adjusted in a way that the emission direction and the kinetic energy after fragmentation lead to variations in the time-of-flight and in the impact position on the detector. Each ion impact creates an electronic signal in the detector; this signal is treated by high-frequency electronics and recorded event by event by a computer. The registered data correspond to the impact times and positions. With these data, the energy and the emission direction of each fragment can be calculated. These values are related to structural properties of the molecule under investigation, i.e. to the bond lengths and relative positions of the atoms, allowing to determine molecule by molecule the handedness of simple chiral species and other isomeric features.

Spin plays a fundamental role in the electronic structure of matter, from single atoms and molecules through to condensed matter. However, spin dynamics and the spin response of electrons to ultra-short, strong laser pulses has remained largely unexplored until today. In 2011 and 2013, pioneering theoretical work [1, 2] extended the fundamental PPT theory [3] to treat ionization of p+ and p” electrons by circular fields. This work predicted the sensitivity of ionization probabilities in strong field ionization using circular fields to the magnetic quantum number, showing that counter rotating electrons can tunnel ionize easier. It also predicted the possibility to obtain spin polarized electrons from strong, circularly polarized fields with a high degree of efficiency. The preference of ionization was later confirmed experimentally by [4], however, the experiment in [4] did not provide a confirmation of the spin polarization predictions.

Citation: McCurdy, C. W., Rescigno, T. N., Trevisan, C. S., Lucchese, R. R., Gaire, B., Menssen, A., . . . Weber, T. (2017). Unambiguous observation of F-atom core-hole localization in CF4 through body-frame photoelectron angular distributions. Physical Review A, 95(1). doi:10.1103/PhysRevA.95.011401

We report on three-dimensional (3D) electron momentum distributions from single ionization of helium by a laser pulse consisting of two counterrotating circularly polarized fields (390 nm and 780 nm). A pronounced 3D low energy structure and sub-cycle interferences are observed experimentally and reproduced numerically using a trajectory based semi-classical simulation. The orientation of the low energy structure in the polarization plane is verified by numerical simulations solving the time dependent Schr\"odinger equation., Comment: 5 pages, 4 figures, PRA Rapid Communications accepted

International Conference on Photonic Electronic and Atomic Collisions 2017, Cairns, Australia, 26 Jul 2017 - 1 Aug 2017; Journal of physics / Conference Series 875, 032009 - (2017). doi:10.1088/1742-6596/875/4/032009, For K-shell ionization of N$_2$ photoelectron auger electron coincident angular distributions show that pathways with gerade and ungerade K-hole state can interfere. On the other hand high resolution photoelectron spectroscopy seems to indicate that the gerade and ungerade hole state can be separated in energy. The present experiment aims to combine the high energy resolution with full angular detection of Auger and Photoelectron to resolve this seeming contradiction., Published by IOP Publ., Bristol

We investigate sequential double ionization of helium by intense near-circularly polarized few-cycle laser pulses using a semiclassical ionization model with two independent electrons. Simulated ${\mathrm{He}}^{2+}$ ion momentum distributions are compared to those obtained in recent benchmark experiments [M. S. Sch\"offler, X. Xie, P. Wustelt, M. M\"oller, S. Roither, D. Kartashov, A. M. Sayler, A. Baltuska, G. G. Paulus, and M. Kitzler, Phys. Rev. A 93, 063421 (2016)]. We study the influence of a number of pulse parameters such as peak intensity, carrier-envelope phase, pulse duration, and second- and third-order spectral phase on the shape of the ion momentum distributions. Good agreement is found in the main features of these distributions and of their dependence on the laser pulse duration, peak intensity, and carrier-envelope phase. Furthermore, we find that for explaining certain fine-scale features observed in the experiments, it becomes important to consider subtle timing variations in the two-electron emissions introduced by small values of chirp. This result highlights the possibility of measuring and controlling multielectron dynamics on the attosecond time scale by fine tuning the field evolution of intense close-to-single-cycle laser pulses.