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- ItemPhotodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization(Melville, NY : AIP Publishing LLC, 2018) Amini, Kasra; Savelyev, Evgeny; Brauße, Felix; Berrah, Nora; Bomme, Cédric; Brouard, Mark; Burt, Michael; Christensen, Lauge; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Kierspel, Thomas; Krecinic, Faruk; Lauer, Alexandra; Lee, Jason W. L.; Müller, Maria; Müller, Erland; Mullins, Terence; Redlin, Harald; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Vallance, Claire; Wiese, Joss; Johnsson, Per; Küpper, Jochen; Rudenko, Artem; Rouzée, Arnaud; Stapelfeldt, Henrik; Rolles, Daniel; Boll, RebeccaWe explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon-iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.
- ItemPhotoelectron holography in strong optical and dc electric fields(Bristol : Institute of Physics Publishing, 2014) Stodolna, A.; Huismans, Y.; Rouzée, A.; Lépine, F.; Vrakking, M.J.J.The application of velocity map imaging for the detection of photoelectrons resulting from atomic or molecular ionization allows the observation of interferometric, and in some cases holographic structures that contain detailed information on the target from which the photoelecrons are extracted. In this contribution we present three recent examples of the use of photoelectron velocity map imaging in experiments where atoms are exposed to strong optical and dc electric fields. We discuss (i) observations of the nodal structure of Stark states of hydrogen measured in a dc electric field, (ii) mid-infrared strong-field ionization of metastable Xe atoms and (iii) the reconstruction of helium electronic wavepackets in an attosecond pump-probe experiment. In each case, the interference between direct and indirect electron pathways, reminiscent of the reference and signal waves in holography, is seen to play an important role.
- ItemCorrelated electronic decay following intense near-infrared ionization of clusters(Bristol : IOP Publ., 2015) Schütte, Bernd; Arbeiter, Mathias; Fennel, Thomas; Jabbari, Ghazal; Kuleff, Alexander I.; Vrakking, Marc J. J.; Rouzée, ArnaudWe report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.
- ItemElectron dynamics in laser-driven atoms near the continuum threshold(Washington, DC : OSA, 2021) Liu, Mingqing; Xu, Songpo; Hu, Shilin; Becker, Wilhelm; Quan, Wei; Liu, Xiaojun; Chen, JingStrong-field ionization and Rydberg-state excitation (RSE) near the continuum threshold exhibit two phenomena that have attracted a lot of recent attention: the low-energy structure (LES) just above and frustrated tunneling ionization just below the threshold. The former becomes apparent for longer laser wavelengths, while the latter has been especially investigated in the near infrared; both have been treated as separate phenomena so far. Here we present a unified perspective based on electron trajectories, which emphasizes the very important role of the electron-ion Coulomb interaction as expected in this energy region. Namely, those trajectories that generate the LES can also be recaptured into a Rydberg state. The coherent superposition of the contributions of such trajectories with different travel times (each generating one of the various LES peaks) causes an oscillation in the intensity dependence of the RSE yield, which is especially noticeable for longer wavelengths. The theory is illustrated by RSE experiments at 1800 nm, which agree very well with the theory with respect to position and period of the oscillation. The wavelength scaling of the RSE oscillation is also discussed. Our work establishes a solid relationship between processes below and above the threshold and sheds new light on atomic dynamics driven by intense laser fields in this critical energy region.
- ItemInterference structure of above-threshold ionization versus above-threshold detachment(Bristol : IOP, 2012) Korneev, Ph.A.; Popruzhenko, S.V.; Goreslavski, S.P.; Becker, W.; Paulus, G.G.; Fetić, B.; Milošević, D.B.Laser-induced electron detachment or ionization of atoms and negative ions is considered. In the context of the saddle-point evaluation of the strong-field approximation (SFA), the velocity maps of the direct electrons (those that do not undergo rescattering) exhibit a characteristic structure due to the constructive and destructive interference of electrons liberated from their parent atoms/ions within certain windows of time. This structure is defined by the above-threshold ionization rings at fixed electron energy and by two sets of curves in momentum space on which destructive interference occurs. The spectra obtained with the SFA are compared with those obtained by numerical solution of the time-dependent Schrödinger equation. For detachment, the agreement is excellent. For ionization, the effect of the Coulomb field is most pronounced for electrons emitted in a direction close to laser polarization, while for nearperpendicular emission the qualitative appearance of the spectrum is unaffected.
- ItemMolecular above-threshold ionization spectra as an evidence of the three-point interference of electron wave packets(Bristol : IOP Publ., 2015) Hasović, Elvedin; Milošević, Dejan B.; Gazibegović-Busuladži, Azra; Čerkić, Aner; Busuladžić, MustafaWe consider high-order above-threshold ionization (HATI) of polyatomic molecules ionized by a strong linearly polarized laser field. Improved molecular strong-field approximation by which the HATI process on polyatomic molecular species can be described is developed. Using this theory we calculate photoelectron angular-energy spectra for different triatomic molecules. Special attention is devoted to the minima that are observed in the calculated high-energy electron spectra of the ozone and carbon dioxide molecules. A key difference between these minima and minima that are observed in the corresponding spectra of diatomic molecules are presented.
- ItemStrong field ionization of small hydrocarbon chains with full 3D momentum analysis(Bristol : IOP Publ., 2015) Schulz, Claus Peter; Birkner, Sascha; Furch, Federico J.; Anderson, Alexandria; Mikosch, Jochen; Schell, Felix; Vrakking, Marc J. J.Strong field ionization of small hydrocarbon chains is studied in a kinematic complete experiment using a reaction microscope. By coincidence detection of ions and electrons different ionization continua populated during the ionization process are identified. In addition, photoelectron momentum distributions from laser-aligned molecules allow to characterize the electron wavepackets emerging from different Dyson orbitals.
- ItemAttosecond electron spectroscopy using a novel interferometric pump-probe technique(College Park, Md. : APS, 2010) Mauritsson, J.; Remetter, T.; Swoboda, M.; Klünder, K.; L'Huillier, A.; Schafer, K.J.; Ghafur, O.; Kelkensberg, F.; Siu, W.; Johnsson, P.; Vrakking, M.J.J.; Znakovskaya, I.; Uphues, T.; Zherebtsov, S.; Kling, M.F.; Lépine, F.; Benedetti, E.; Ferrari, F.; Sansone, G.; Nisoli, M.We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse (AP) with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original AP. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multipath interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the AP duration. © 2010 The American Physical Society.
- ItemIntracycle interference in ionization of Ar by a laser assisted XUV pulse(Bristol : IOP Publ., 2017) Arbó, D.G.; López, S. D.; Kubin, M.; Hummert, J.; Vrakking, M.J.J.; Kornilov, O.Synopsis We present a theoretical and experimental study of the subcycle interference in laser assisted XUV ionization of Ar atoms. Averaging over the focal volume happens to blur the intracycle interference, which thus cannot be measured directly. We show that even at these conditions, the intracycle interference can be obtained through the subtraction of two different angle and energy-resolved distributions at slightly different laser intensities.
- ItemReconstruction of the time-dependent electronic wave packet arising from molecular autoionization(Washington, DC [u.a.] : Assoc., 2018) Bello, Roger Y.; Canton, Sophie E.; Jelovina, Denis; Bozek, John D.; Rude, Bruce; Smirnova, Olga; Ivanov, Mikhail Y.; Palacios, Alicia; Martín, FernandoAutoionizing resonances are paradigmatic examples of two-path wave interferences between direct photoionization, which takes a few attoseconds, and ionization via quasi-bound states, which takes much longer. Time-resolving the evolution of these interferences has been a long-standing goal, achieved recently in the helium atom owing to progress in attosecond technologies. However, already for the hydrogen molecule, similar time imaging has remained beyond reach due to the complex interplay between fast nuclear and electronic motions. We show how vibrationally resolved photoelectron spectra of H2 allow one to reconstruct the associated subfemtosecond autoionization dynamics by using the ultrafast nuclear dynamics as an internal clock, thus forgoing ultrashort pulses. Our procedure should be general for autoionization dynamics in molecules containing light nuclei, which are ubiquitous in chemistry and biology.