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Tamás Csizmadia

Publications and source records attributed to Tamás Csizmadia.

10 recordsLinked to original sources

Breakdown of the isotropic asymptotic approximation in two-colour photoionisation

The Wigner delay is defined as the energy derivative of the scattering phase of a particle in a given potential, unveiling the time taken (or gained) due to the interaction. The characterisation of this delay plays a central role in attosecond science, where the time resolution allows to gain information on the time interval required for a photoelectron to be emitted into the continuum after the absorption of a single photon. Attosecond interferometric techniques, based on two-colour (extreme ultraviolet and near-infrared) photoionisation schemes, cannot provide a direct measurement of the Wigner delay, because the low-frequency photon contributes with an additional delay, which is imprinted on the outgoing photoelectron. The isolation of the Wigner delay is usually achieved by appealing to the asymptotic approximation, which assumes that the two-photon delay is separable into a Wigner and a near-infrared-induced phase and provides a universal analytical expression for the latter. In this study, we introduce a self-referencing approach based on the implementation of non-consecutive extreme ultraviolet harmonics, in order to test the validity of the asymptotic approximation. We demonstrate its breakdown by observing a deviation of a few tens of milliradians (corresponding to a few attoseconds) between its predictions and the experimentally measured phases of the sideband oscillations generated in our scheme, in agreement with full-dimensional simulations.

physics.atom-ph↗

Active stabilization for ultralong acquisitions in an attosecond pump-probe beamline

Attosecond time-resolution experiments using noncollinear interferometers require precise and active control of the optical delay to prevent instabilities - including both slow drifts and rapid vibrations - that can obscure the time evolution of the physical system under investigation. In this work, we present the design and results of stability measurements for a double interferometer setup for extreme ultraviolet-infrared pump-probe spectroscopy. The attosecond pump-probe setup is driven by a high-average-power, high-repetition-rate laser system and offers sub-optical-cycle (+/-81 as) stability with a fast feedback rate over extended periods (up to several days). Due to the noncollinear arrangement, the setup enables independent control of both amplitude and phase in the two arms even across significantly different spectral regions. As a proof of concept, we demonstrate attosecond beating in angle-resolved photoemission during two-photon, two-color photoionization, highlighting the broad potential of the system for kinematically and dynamically complete studies of atomic-scale light-matter interactions.

physics.optics↗

Spectrally tunable ultrashort monochromatized extreme ultraviolet pulses at 100 kHz

We present the experimental realization of spectrally tunable, ultrashort, quasi-monochromatic extreme ultraviolet (XUV) pulses generated at 100 kHz repetition rate in a user-oriented gas high harmonic generation (GHHG) beamline of the Extreme Light Infrastructure - Attosecond Light Pulse Source (ELI ALPS) facility. Versatile spectral and temporal shaping of the XUV pulses are accomplished with a double-grating, time-delay compensated monochromator accommodating the two composing stages in a novel, asymmetrical geometry. This configuration supports the achievement of high monochromatic XUV flux (2.8+/-0.9*1e10 photons/s at 39.7 eV selected with 700 meV FWHM bandwidth) combined with ultrashort pulse duration (4.0+/-0.2 fs using 12.1+/-0.6 fs driving pulses) and small spot size (sub-100 um). Focusability, spectral bandwidth, and overall photon flux of the produced radiation were investigated covering a wide range of instrumental configurations. Moreover, complete temporal (intensity and phase) characterization of the few-femtosecond monochromatic XUV pulses - a goal that is difficult to achieve by conventional reconstruction techniques - has been realized using ptychographic algorithm on experimentally recorded XUV-IR pump-probe traces. The presented results contribute to in-situ, time-resolved experiments accessing direct information on the electronic structure dynamics of novel target materials.

physics.optics↗

Liquid-cooled modular gas cell system for high-order harmonic generation using high average power laser systems

We present the design and implementation of a new, modular gas target suitable for high-order harmonic generation using high average power lasers. To ensure thermal stability in this high heat load environment, we implement an appropriate liquid cooling system. The system can be used in multiple-cell configurations allowing to control the cell length and aperture size. The cell design was optimized with heat and flow simulations for thermal characteristics, vacuum compatibility and generation medium properties. Finally, the cell system was experimentally validated by conducting high-order harmonic generation measurements using the 100 kHz high average power HR-1 laser system at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI ALPS) facility. Such a robust, versatile and stackable gas cell arrangement can easily be adapted to different experimental geometries in both table-top laboratory systems and user-oriented facilities, such as ELI ALPS.

physics.ins-det↗

Detailed study of quantum path interferences in high harmonic generation driven by chirped laser pulses

We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control parameters of such a driving laser pulse influencing the high harmonic spectra. Specifically, the impact of the pulse duration, peak intensity and instantaneous frequency is studied in a self-consistent manner based on Lewenstein formalism. Simulations involving macroscopic propagation effects are also considered. The study aims to reveal the microscopic background behind a variety of interference patterns capturing important information both about the fundamental laser field and the generation process itself. The results provide guidance towards experiments with chirp control as a tool to unravel, explain and utilize the rich and complex interplay between quantum path interferences including the tuning of the periodicity of the intensity dependent oscillation of the harmonic signal, and the curvature of spectrally resolved Maker fringes.

physics.atom-ph↗

High-flux 100-kHz attosecond pulse source driven by a high average power annular laser beam

High-repetition-rate attosecond pulse sources are indispensable tools of time-resolved studies of electron dynamics, such as coincidence spectroscopy and experiments with high demands on statistics or signal-to-noise ratio, especially in case of solid and big molecule samples in chemistry and biology. Although with the high-repetition-rate lasers such attosecond pulses in a pump-probe configuration are possible to achieve, until now only a few such light sources have been demonstrated. Here, by shaping the driving laser to an annular beam, a 100-kHz attosecond pulse train (APT) is reported with the highest energy so far (51 pJ/shot) on target (269 pJ at generation) among the high-repetition-rate systems (> 10 kHz) in which the attosecond pulses were temporally characterized. The on-target pulse energy is maximized by reducing the losses from the reflections and filtering of the high harmonics, and an unprecedented 19% transmission rate from the generation point to the target position is achieved. At the same time, the probe beam is also annular, and low loss of this beam is reached by using another holey mirror to combine with the APT. The advantages of using an annular beam to generate attosecond pulses with a high average power laser is demonstrated experimentally and theoretically. The effect of nonlinear propagation in the generation medium on the annular-beam generation concept is also analyzed in detail.

physics.optics↗

All-Optical Experimental Control of High-Harmonic Photon Energy

We generate high-order harmonics in gaseous medium with tunable photon energy using time domain interferometry of double pulses in a non-collinear generation geometry. The method is based on the fact that the generated harmonics inherit certain spectral properties of the driving laser. The two temporally delayed ultrashort laser pulses, identical in all parameters, are produced by a custom-made split-and-delay unit utilizing wave front splitting without a significant energy loss. The arrangement is easy to implement in any attosecond pulse generation beamline, and is suitable for the production of an extreme ultraviolet source with simply and quickly variable central photon energy, useful for a broad range of applications.

physics.optics↗

Attosecond Pulse-shaping using a seeded free-electron laser

Attosecond pulses are fundamental for the investigation of valence and core-electron dynamics on their natural timescale. At present the reproducible generation and characterisation of attosecond waveforms has been demonstrated only through the process of high-order harmonic generation. Several methods for the shaping of attosecond waveforms have been proposed, including metallic filters, multilayer mirrors and manipulation of the driving field. However, none of these approaches allow for the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free Electron Lasers, on the contrary, deliver femtosecond, extreme ultraviolet and X-ray pulses with energies ranging from tens of $\mathrmμ$J to a few mJ. Recent experiments have shown that they can generate sub-fs spikes, but with temporal characteristics that change shot-to-shot. Here we show the first demonstration of reproducible generation of high energy ($\mathrmμ$J level) attosecond waveforms using a seeded Free Electron Laser. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with a novel approach for its temporal reconstruction. The results presented here open the way to perform attosecond time-resolved experiments with Free Electron Lasers.

physics.optics↗

A new method for measuring angle-resolved phases in photoemission

Quantum mechanically, photoionization can be fully described by the complex photoionization amplitudes that describe the transition between the ground state and the continuum state. Knowledge of the value of the phase of these amplitudes has been a central interest in photoionization studies and newly developing attosecond science, since the phase can reveal important information about phenomena such as electron correlation. We present a new attosecond-precision interferometric method of angle-resolved measurement for the phase of the photoionization amplitudes, using two phase-locked Extreme Ultraviolet pulses of frequency $ω$ and $2ω$, from a Free-Electron Laser. Phase differences $Δ\tilde η$ between one- and two-photon ionization channels, averaged over multiple wave packets, are extracted for neon $2p$ electrons as a function of emission angle at photoelectron energies 7.9, 10.2, and 16.6 eV. $Δ\tilde η$ is nearly constant for emission parallel to the electric vector but increases at 10.2 eV for emission perpendicular to the electric vector. We model our observations with both perturbation and \textit{ab initio} theory, and find excellent agreement. In the existing method for attosecond measurement, Reconstruction of Attosecond Beating By Interference of Two-photon Transitions (RABBITT), a phase difference between two-photon pathways involving absorption and emission of an infrared photon is extracted. Our method can be used for extraction of a phase difference between single-photon and two-photon pathways and provides a new tool for attosecond science, which is complementary to RABBITT.

physics.atom-ph↗

Generation of high-order harmonics with tunable photon energy and spectral width using double pulses

This work theoretically investigates high-order harmonic generation in rare gas atoms driven by two temporally delayed ultrashort laser pulses. Apart from their temporal delay, the two pulses are identical. Using a single-atom model of the laser-matter interaction it is shown that the photon energy of the generated harmonics is controllable within the range of one eV -- a bandwidth comparable to the photon energy of the fundamental field -- by varying the time delay between the generating laser pulses. It is also demonstrated that high-order harmonics generated by double pulses have advantageous characteristics, which mimick certain properties of an extreme ultraviolet (XUV) monochromator. With the proposed method, a simpler setup at a much lower cost and comparatively higher spectral yield can be implemented in contrast to other approaches.

physics.optics↗