| 1. |
- 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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| 2. |
- 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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| 3. |
- 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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| 4. |
- 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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| 5. |
- 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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| 6. |
- 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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| 7. |
- 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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| 8. |
- Milli, J., et al.
(författare)
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Near-infrared scattered light properties of the HR4796A dust ring A measured scattering phase function from 13.6 degrees to 166.6 degrees
- 2017
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Ingår i: Astronomy and Astrophysics. - : EDP Sciences. - 0004-6361 .- 1432-0746. ; 599
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Tidskriftsartikel (refereegranskat)abstract
- Context. HR4796A is surrounded by a debris disc, observed in scattered light as an inclined ring with a high surface brightness. Past observations have raised several questions. First, a strong brightness asymmetry detected in polarised reflected light has recently challenged our understanding of scattering by the dust particles in this system. Secondly, the morphology of the ring strongly suggests the presence of planets, although no planets have been detected to date.Aims. We aim here at measuring with high accuracy the morphology and photometry of the ring in scattered light, in order to derive the phase function of the dust and constrain its near-infrared spectral properties. We also want to constrain the presence of planets and set improved constraints on the origin of the observed ring morphology.Methods. We obtained high-angular resolution coronagraphic images of the circumstellar environment around HR4796A with VLT/SPHERE during the commissioning of the instrument in May 2014 and during guaranteed-time observations in February 2015. The observations reveal for the first time the entire ring of dust, including the semi-minor axis that was previously hidden either behind the coronagraphic spot or in the speckle noise.Results. We determine empirically the scattering phase function of the dust in the H band from 13.6 degrees to 166.6 degrees. It shows a prominent peak of forward scattering, never detected before, for scattering angles below 30 degrees. We analyse the reflectance spectra of the disc from the 0.95 mu m to 1.6 mu m, confirming the red colour of the dust, and derive detection limits on the presence of planetary mass objects.Conclusions. We confirm which side of the disc is inclined towards the Earth. The analysis of the phase function, especially below 45 degrees, suggests that the dust population is dominated by particles much larger than the observation wavelength, of about 20 mu m. Compact Mie grains of this size are incompatible with the spectral energy distribution of the disc, however the observed rise in scattering efficiency beyond 50 degrees points towards aggregates which could reconcile both observables. We do not detect companions orbiting the star, but our high-contrast observations provide the most stringent constraints yet on the presence of planets responsible for the morphology of the dust.
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| 9. |
- Patchkovskii, Serguei, et al.
(författare)
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Theory of nuclear motion in RABBITT spectra
- 2023
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Ingår i: Physical Review A. - 2469-9926. ; 107:4
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Tidskriftsartikel (refereegranskat)abstract
- Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is a powerful photoelectron spectroscopy, offering direct access to internal dynamics of the target. It is being increasingly applied to molecular systems, but a general, computationally tractable theory of RABBITT spectra in molecules has so far been lacking. We show that under quite general assumptions, RABBITT spectra in molecules can be expressed as a convolution of the vibronic cross-correlation functions and two-electron photoionization matrix elements. We specialize the general expressions to the commonly encountered special cases. We expect our theory to enable accurate modeling and interpretation of molecular RABBITT spectra in most medium-sized molecules.
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