| 1. |
- Kumar Maroju, Praveen, et al.
(författare)
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Attosecond pulse shaping using a seeded free-electron laser
- 2020
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 578, s. 386-391
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Tidskriftsartikel (refereegranskat)abstract
- Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales. The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation. Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters, multilayer mirrors and manipulation of the driving field. However, none of these approaches allows 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, by contrast, deliver femtosecond, extreme-ultraviolet and X-ray pulses with energies ranging from tens of microjoules to a few millijoules. Recent experiments have shown that they can generate subfemtosecond spikes, but with temporal characteristics that change shot-to-shot. Here we report reproducible generation of high-energy (microjoule 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 an approach for its temporal reconstruction. The results presented here open the way to performing attosecond time-resolved experiments with free-electron lasers.
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| 2. |
- Maroju, Praveen K., et al.
(författare)
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A Novel Attosecond Timing Tool for Free-Electron Laser Experiment
- 2020
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Ingår i: High Intensity Lasers and High Field Phenomena 2020. - 9781943580736
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Konferensbidrag (refereegranskat)abstract
- We demonstrate a novel timing tool for Free-Electron Lasers to determine the delay between an attosecond pulse train and infrared pulse with sub-optical-cycle resolu-. tion.
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| 3. |
- Wituschek, Andreas, et al.
(författare)
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Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses
- 2020
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 11
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Tidskriftsartikel (refereegranskat)abstract
- The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths.
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| 4. |
- Callegari, Carlo, et al.
(författare)
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Application of matched-filter concepts to unbiased selection of data in pump-probe experiments with free electron lasers
- 2017
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Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 7:6
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Tidskriftsartikel (refereegranskat)abstract
- Pump-probe experiments are commonly used at Free Electron Lasers (FEL) to elucidate the femtosecond dynamics of atoms, molecules, clusters, liquids and solids. Maximizing the signal-to-noise ratio of the measurements is often a primary need of the experiment, and the aggregation of repeated, rapid, scans of the pump-probe delay is preferable to a single long-lasting scan. The limited availability of beamtime makes it impractical to repeat measurements indiscriminately, and the large, rapid flow of single-shot data that need to be processed and aggregated into a dataset, makes it difficult to assess the quality of a measurement in real time. In post-analysis it is then necessary to devise unbiased criteria to select or reject datasets, and to assign the weight with which they enter the analysis. One such case was the measurement of the lifetime of Intermolecular Coulombic Decay in the weakly-bound neon dimer. We report on the method we used to accomplish this goal for the pump-probe delay scans that constitute the core of the measurement; namely we report on the use of simple auto- and cross-correlation techniques based on the general concept of "matched filter". We are able to unambiguously assess the signal-to-noise ratio (SNR) of each scan, which then becomes the weight with which a scan enters the average of multiple scans. We also observe a clear gap in the values of SNR, and we discard all the scans below a SNR of 0.45. We are able to generate an average delay scan profile, suitable for further analysis: in our previous work we used it for comparison with theory. Here we argue that the method is sufficiently simple and devoid of human action to be applicable not only in post-analysis, but also for the real-time assessment of the quality of a dataset.
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| 5. |
- Charalambidis, Dimitris, et al.
(författare)
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The extreme light infrastructure—attosecond light pulse source (ELI-ALPS) project
- 2017. - 9783319648392
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Ingår i: Springer Series in Chemical Physics. - Cham : Springer International Publishing. - 0172-6218. ; :9783319648392, s. 181-218
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Bokkapitel (refereegranskat)abstract
- Globally, large international research infrastructures have over many decades promoted excellence in science and technology. Aligned with the international practice, the Europe Strategy Forum for Research Infrastructures (ESFRI) has developed and keeps updating a roadmap for research infrastructures. The Extreme Light Infrastructure (ELI) is one of the two large scale Laser Research Infrastructures (RI) proposed in the ESFRI Roadmap published in 2006. ELI aims to provide access to some of the most intense world-wide lasers for the international scientific user community, as well as secondary radiation and particle sources driven by them, offering to the users new interdisciplinary research opportunities. ELI is currently implemented as a distributed infrastructure in three pillars: ELI-Beamlines (ELI-BL) in Dolní Břežany, Czech Republic, ELI-Attosecond Light Pulse Source (ELI-ALPS) in Szeged, Hungary and ELI-Nuclear Physics (ELI-NP) in Magurele, Romania. This chapter is devoted to introduce the Hungarian pillar, ELI-ALPS, which will be operational in Szeged in 2018, with the primary mission to provide to the users the highest laboratory spatiotemporal resolution and a secondary mission to contribute to the technological development towards 200 petawatt (PW) lasers for high-field science, which is the ultimate goal of the ELI project. The chapter includes descriptions of the primary and secondary sources, while emphasis is given to selected examples of the scientific case of ELI-ALPS, presenting unique access offered by the technologies to be hosted in the infrastructure.
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| 6. |
- Ertel, Dominik, et al.
(författare)
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Anisotropy Parameters for Two-Color Photoionization Phases in Randomly Oriented Molecules : Theory and Experiment in Methane and Deuteromethane
- 2024
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Ingår i: Journal of Physical Chemistry A. - 1089-5639 .- 1520-5215. ; 128:9, s. 1685-1697
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Tidskriftsartikel (refereegranskat)abstract
- We present combined theoretical and experimental work investigating the angle-resolved phases of the photoionization process driven by a two-color field consisting of an attosecond pulse train and an infrared pulse in an ensemble of randomly oriented molecules. We derive a general form for the two-color photoelectron (and time-delay) angular distribution valid also in the case of chiral molecules and when relative polarizations of the photons contributing to the attosecond photoelectron interferometer differ. We show a comparison between the experimental data and theoretical predictions in an ensemble of methane and deuteromethane molecules, discussing the effect of nuclear dynamics on the photoionization phases. Finally, we demonstrate that the oscillating component and the phase of the two-color signal can be fitted by using complex asymmetry parameters, in perfect analogy to the atomic case.
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| 7. |
- Ertel, Dominik, et al.
(författare)
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Influence of nuclear dynamics on molecular attosecond photoelectron interferometry
- 2023
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Ingår i: Science Advances. - 2375-2548. ; 9:35
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Tidskriftsartikel (refereegranskat)abstract
- In extreme ultraviolet spectroscopy, the photoionization process occurring in a molecule due to the absorption of a single photon can trigger an ultrafast nuclear motion in the cation. Taking advantage of attosecond photoelectron interferometry, where the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional infrared quantum of light, one can investigate the influence of nuclear dynamics by monitoring the characteristics of the photoelectron spectra generated by the two-color field. Here, we show that attosecond photoelectron interferometry is sensitive to the nuclear response by measuring the two-color photoionization spectra in a mixture of methane (CH4) and deuteromethane (CD4). The effect of the different nuclear evolution in the two isotopologues manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks. Our work indicates that nuclear dynamics can affect the coherence properties of the electronic wave packet emitted by photoionization on a time scale as short as a few femtoseconds.
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| 8. |
- Fushitani, Mizuho, et al.
(författare)
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Time-resolved photoelectron imaging of complex resonances in molecular nitrogen
- 2021
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Ingår i: The Journal of chemical physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 154:14
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Tidskriftsartikel (refereegranskat)abstract
- We have used the FERMI free-electron laser to perform time-resolved photoelectron imaging experiments on a complex group of resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, N2, under jet-cooled conditions. The new data complement and extend the earlier work of Fushitani et al. [Opt. Express 27, 19702–19711 (2019)], who recorded time-resolved photoelectron spectra for this same group of resonances. Time-dependent oscillations are observed in both the photoelectron yields and the photoelectron angular distributions, providing insight into the interactions among the resonant intermediate states. In addition, for most states, we observe an exponential decay of the photoelectron yield that depends on the ionic final state. This observation can be rationalized by the different lifetimes for the intermediate states contributing to a particular ionization channel. Although there are nine resonances within the group, we show that by detecting individual photoelectron final states and their angular dependence, we can identify and differentiate quantum pathways within this complex system.
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| 9. |
- Fushitani, Mizuho, et al.
(författare)
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Wave packet dynamics and control in excited states of molecular nitrogen
- 2024
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Ingår i: The Journal of chemical physics. - 0021-9606. ; 160:10
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Tidskriftsartikel (refereegranskat)abstract
- Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N2. Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ∼ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.
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| 10. |
- Kühn, Sergei, et al.
(författare)
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The ELI-ALPS facility : The next generation of attosecond sources
- 2017
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 50:13
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Forskningsöversikt (refereegranskat)abstract
- This review presents the technological infrastructure that will be available at the Extreme Light Infrastructure Attosecond Light Pulse Source (ELI-ALPS) international facility. ELI-ALPS will offer to the international scientific community ultrashort pulses in the femtosecond and attosecond domain for time-resolved investigations with unprecedented levels of high quality characteristics. The laser sources and the attosecond beamlines available at the facility will make attosecond technology accessible for scientists lacking access to these novel tools. Time-resolved investigation of systems of increasing complexity is envisaged using the end stations that will be provided at the facility.
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| 11. |
- Maroju, Praveen Kumar, et al.
(författare)
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Complex attosecond waveform synthesis at fel fermi
- 2021
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Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 11:21
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Tidskriftsartikel (refereegranskat)abstract
- Free-electron lasers (FELs) can produce radiation in the short wavelength range extending from the extreme ultraviolet (XUV) to the X-rays with a few to a few tens of femtoseconds pulse duration. These facilities have enabled significant breakthroughs in the field of atomic, molecular, and optical physics, implementing different schemes based on two-color photoionization mechanisms. In this article, we present the generation of attosecond pulse trains (APTs) at the seeded FEL FERMI using the beating of multiple phase-locked harmonics. We demonstrate the complex attosecond waveform shaping of the generated APTs, exploiting the ability to manipulate independently the amplitudes and the phases of the harmonics. The described generalized attosecond waveform synthesis technique with an arbitrary number of phase-locked harmonics will allow the generation of sub-100 as pulses with programmable electric fields.
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| 12. |
- Nayak, Arjun, et al.
(författare)
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Saddle point approaches in strong field physics and generation of attosecond pulses
- 2019
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Ingår i: Physics Reports. - : Elsevier BV. - 0370-1573. ; 833, s. 1-52
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Forskningsöversikt (refereegranskat)abstract
- Attoscience is the emerging field that accesses the fastest electronic processes occurring at the atomic and molecular length scales with attosecond (1 as = 10−18 s) time resolution having wide ranging physical, chemical, material science and biological applications. The quintessential and one of the most fundamental processes in this domain is the generation of phase locked XUV attosecond pulses. The theoretical approach to understand the process incorporates a fully quantum or semi classical or relativistic description of coherent charge dynamics in intense ultrashort electromagnetic fields driving a quantum system (an atom, a molecule, solid band gap materials or surface plasmas). Modelling of such physical and dynamical systems in science and also in many other branches often leads to equations represented in terms of complex multi-dimensional integrals. These integrals can often be solved using the stationary phase approximation, which leads to a series of equations identifying the points in the multi-dimensional space, having most significant contributions in their evaluation. These points are usually indicated as saddle points. The description of the dynamics of quantum mechanical or relativistic systems that results from such an approach enables near to classical physics intuitive perceptions of the processes under investigation. Thus, the saddle point methods are very powerful and valuable general theoretical tools to obtain asymptotic expressions of such solutions and help also to gain physical insights on the underlying phenomena. Such techniques developed in the past have been adapted to study the emission of as pulses by different physical systems and have been widely employed in calculating and estimating the response of matter to intense electromagnetic pulses on ultrafast time scales. Here we provide an extensive disposition of the saddle point approaches unifying their ubiquitous applications within the domain of attoscience valid for simple atomic to more complex condensed matter systems undergoing ultrafast dynamics and present current trends and advancements in the field. In this review we would delineate the methodology, present a synthesis of seminal works and describe the state of the art applications. Finally we also address ultrashort time dynamics of novel materials that have gained much attention recently, namely lower dimensional material systems and micro-plasma systems.
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| 13. |
- Ueda, Kiyoshi, et al.
(författare)
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Roadmap on photonic, electronic and atomic collision physics : I. Light-matter interaction
- 2019
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Ingår i: Journal of Physics B. - : IOP PUBLISHING LTD. - 0953-4075 .- 1361-6455. ; 52:17
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Tidskriftsartikel (refereegranskat)abstract
- We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light-matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field.
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