13 results
Search Results
Now showing 1 - 10 of 13
- ItemDiffraction imaging of light induced dynamics in xenon-doped helium nanodroplets([London] : IOP, 2022-11-30) Langbehn, B.; Ovcharenko, Y.; Clark, A.; Coreno, M.; Cucini, R.; Demidovich, A.; Drabbels, M.; Finetti, P.; Di Fraia, M.; Giannessi, L.; Grazioli, C.; Iablonskyi, D.; LaForge, A.C.; Nishiyama, T.; Oliver Álvarez de Lara, V.; Peltz, C.; Piseri, P.; Plekan, O.; Sander, K.; Ueda, K.; Fennel, T.; Prince, K.C.; Stienkemeier, F.; Callegari, C.; Möller, T.; Rupp, D.We explore the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump–probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation with near-infrared laser pulses. After a variable time delay of up to 800 ps, we image the subsequent dynamics using intense extreme ultraviolet pulses from the FERMI free-electron laser. The recorded scattering images exhibit complex intensity fluctuations that are categorized based on their characteristic features. Systematic simulations of wide-angle diffraction patterns are performed, which can qualitatively explain the observed features by employing model shapes with both randomly distributed as well as structured, symmetric distortions. This points to a connection between the dynamics and the positions of the dopants in the droplets. In particular, the structured fluctuations might be governed by an underlying array of quantized vortices in the superfluid droplet as has been observed in previous small-angle diffraction experiments. Our results provide a basis for further investigations of dopant–droplet interactions and associated heating mechanisms.
- ItemFemtosecond XUV–IR induced photodynamics in the methyl iodide cation([London] : IOP, 2021) Murillo-Sánchez, Marta L.; Reitsma, Geert; Poullain, Sonia Marggi; Fernández-Milán, Pedro; González-Vázquez, Jesús; de Nalda, Rebeca; Martín, Fernando; Vrakking, Marc J. J.; Kornilov, Oleg; Bañares, LuisThe time-resolved photodynamics of the methyl iodide cation (CH3I+) are investigated by means of femtosecond XUV-IR pump-probe spectroscopy. A time-delay-compensated XUV monochromator is employed to isolate a specific harmonic, the 9th harmonic of the fundamental 800 nm (13.95 eV, 88.89 nm), which is used as a pump pulse to prepare the cation in several electronic states. A time-delayed IR probe pulse is used to probe the dissociative dynamics on the first excited state potential energy surface. Photoelectrons and photofragment ions - and I+ - are detected by velocity map imaging. The experimental results are complemented with high level ab initio calculations for the potential energy curves of the electronic states of CH3I+ as well as with full dimension on-the-fly trajectory calculations on the first electronically excited state, considering the presence of the IR pulse. The and I+ pump-probe transients reflect the role of the IR pulse in controlling the photodynamics of CH3I+ in the state, mainly through the coupling to the ground state and to the excited state manifold. Oscillatory features are observed and attributed to a vibrational wave packet prepared in the state. The IR probe pulse induces a coupling between electronic states leading to a slow depletion of fragments after the cation is transferred to the ground states and an enhancement of I+ fragments by absorption of IR photons yielding dissociative photoionization. © 2021 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.
- ItemLaser stripping of hydrogen atoms by direct ionization([London] : IOP, 2015) Brunetti, E.; Becker, W.; Bryant, H.C.; Jaroszynski, D.A.; Chou, W.Direct ionization of hydrogen atoms by laser irradiation is investigated as a potential new scheme to generate proton beams without stripping foils. The time-dependent Schrödinger equation describing the atom-radiation interaction is numerically solved obtaining accurate ionization cross-sections for a broad range of laser wavelengths, durations and energies. Parameters are identified where the Doppler frequency up-shift of radiation colliding with relativistic particles can lead to efficient ionization over large volumes and broad bandwidths using currently available lasers.
- ItemCorrigendum: Generation of high-quality GeV-class electron beams utilizing attosecond ionization injection (2021 New J. Phys. 23 043016)([London] : IOP, 2021) Lécz, Zsolt; Andreev, Alexander; Kamperidis, C.; Hafz, NasrAcceleration of electrons in laser-driven plasma wakefields has been extended up to the ∼8 GeV energy within a distance of tens of centimeters. However, in applications, requiring small energy spread within the electron bunch, only a small portion of the bunch can be used and often the low-energy electrons represent undesired background in the spectrum. We present a compact and tunable scheme providing clean and mono-energetic electron bunches with less than one percent energy spread and with central energy on the GeV level. It is a two-step process consisting of ionization injection with attosecond pulses and acceleration in a capillary plasma wave-guide. Semi-analytical theory and particle-in-cell simulations are used to accurately model the injection and acceleration steps.
- ItemSub-laser-cycle control of coupled electron–nuclear dynamics at a conical intersection([London] : IOP, 2015) Richter, Maria; Bouakline, Foudhil; González-Vázquez, Jesús; Martínez-Fernández, Lara; Corral, Inés; Patchkovskii, Serguei; Morales, Felipe; Ivanov, Misha; Martín, Fernando; Smirnova, OlgaNonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electron–nuclear dynamics at CIs, offered by the advent of nearly single-cycle, phase-stable, mid-infrared laser pulses. To illustrate the control mechanism, a two-dimensional model of the NO2 molecule is considered. The key idea of the control scheme is to match the time scale of the laser field oscillations to the characteristic time scale of the wave packet transit through the CI. The instantaneous laser field changes the shape and position of the CI as the wave packet passes through. As the CI moves in the laser field, it 'slices' through the wave packet, sculpting it in the coordinate and momentum space in a way that is sensitive to the carrier-envelope phase of the control pulse. We find that the electronic coherence imparted on the sub-laser-cycle time scale manifests during much longer nuclear dynamics that follow on the many tens of femtosecond time scale. Control efficiency as a function of molecular orientation is analyzed, showing that modest alignment is sufficient for showing the described effects.
- ItemSignatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versusab initiocalculations([London] : IOP, 2015) Medišauskas, Lukas; Morales, Felipe; Palacios, Alicia; González-Castrillo, Alberto; Plimak, Lev; Smirnova, Olga; Martín, Fernando; Ivanov, Misha YuWe present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals.
- ItemPhase cycling of extreme ultraviolet pulse sequences generated in rare gases([London] : IOP, 2020) Wituschek, Andreas; Kornilov, Oleg; Witting, Tobias; Maikowski, Laura; Stienkemeier, Frank; Vrakking, Marc J.J.; Bruder, LukasThe development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics (˜14 eV) in argon and krypton. Our technique simultaneously provides high phase stability and a pathway-selective detection scheme for nonlinear signals - both necessary prerequisites for all types of coherent nonlinear spectroscopy. © 2020 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.
- ItemTerahertz pulse generation by two-color laser fields with circular polarization([London] : IOP, 2020) Tailliez, C.; Stathopulos, A.; Skupin, S.; Buožius, D.; Babushkin, T.; Vaičaitis, I.; Bergé, L.We study the influence of the polarization states of ionizing femtosecond two-color pulses on the emitted terahertz radiation in gases. A local-current model and plane-wave evaluations justify the previously-reported impact on the THz energy yield and a (almost) linearly-polarized THz field when using circularly-polarized laser harmonics. For such pump pulses, the THz yield is independent of the relative phase between the two colors. When the pump pulses have same helicity, the increase in the THz yield is associated with longer ionization sequences and higher electron transverse momenta acquired in the driving field. Reversely, for two color pulses with opposite helicity, the dramatic loss of THz power comes from destructive interferences driven by the highly symmetric response of the photocurrents lined up on the third harmonic of the fundamental pulse. While our experiments confirm an increased THz yield for circularly-polarized pumps of same helicity, surprisingly, the emitted THz radiation is not linearly-polarized. This effect is explained by means of comprehensive 3D numerical simulations highlighting the role of the spatial alignment and non-collinear propagation of the two colors. © 2020 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.
- ItemHighly efficient XUV generation via high-order frequency mixing([London] : IOP, 2020) Khokhlova, M.A.; Strelkov, V.V.The efficient generation of the coherent XUV light via frequency conversion of intense laser drivers is a problem of both fundamental and technological importance. Increasing the intensity of the generated high harmonics by raising the intensity of the driving field works only up to a point: at high intensities, rapid ionisation of the medium limits the conversion efficiency. Considering the combined effect of the phase-matching and of the blue shift of the driving field during its propagation in a rapidly ionising medium, we show that the latter can be the dominant limiting mechanism. We introduce a new spatial scale, the blue-shift length, which sets the upper bound for the quadratic intensity growth of the generated harmonics. Moreover, we show that this seemingly fundamental restriction can be overcome by using an additional generating weak mid-IR field. For specific combinations of frequencies of the generating fields, the corresponding high-order frequency-mixing process does not suffer from the blue shift of the drivers and phase mismatch, and thus its efficiency grows quadratically with propagation distance. Our results thus open a new route for highly efficient generation of coherent XUV light. © 2020 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.
- ItemTwo-particle quantum correlations in stochastically-coupled networks([London] : IOP, 2019) de J León-Montiel, Roberto; Méndez, Vicenç; Quiroz-Juárez, Mario A.; Ortega, Adrian; Benet, Luis; Perez-Leija, Armando; Busch, KurtQuantum walks in dynamically-disordered networks have become an invaluable tool for understanding the physics of open quantum systems. Although much work has been carried out considering networks affected by diagonal disorder, it is of fundamental importance to study the effects of fluctuating couplings. This is particularly relevant in materials science models, where the interaction forces may change depending on the species of the atoms being linked. In this work, we make use of stochastic calculus to derive a master equation for the dynamics of one and two non-interacting correlated particles in tight-binding networks affected by off-diagonal dynamical disorder. We show that the presence of noise in the couplings of a quantum network creates a pure-dephasing-like process that destroys all coherences in the single-particle Hilbert subspace. Moreover, we show that when two or more correlated particles propagate in the network, coherences accounting for particle indistinguishability are robust against the impact of off-diagonal noise, thus showing that it is possible, in principle, to find specific conditions for which many indistinguishable particles can traverse stochastically-coupled networks without losing their ability to interfere. © 2019 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.