| 1. |
- Arnold, Cord L., et al.
(författare)
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A high-repetition rate attosecond pulse source for coincidence spectroscopy
- 2021
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Ingår i: 2021 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2021. - 9781665418768
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Konferensbidrag (refereegranskat)abstract
- The power of attosecond pump-probe spectroscopy combined with advanced detection schemes, such as photoelectron/ion coincidence spectrometers and time-resolved photoelectron emission microscopy (PEEM), can be unleashed by properly accounting for the repetition rate of the source. In this work, we present a high-repetition rate (200 kHz) attosecond pulse source that opens up for exploring phenomena, previously inaccessible to the community using attosecond interferometric and spectroscopy pump-probe techniques [1].
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| 2. |
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| 3. |
- Busto, David, et al.
(författare)
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Fano's Propensity Rule in Angle-Resolved Attosecond Pump-Probe Photoionization
- 2019
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 123:13
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Tidskriftsartikel (refereegranskat)abstract
- In a seminal article, Fano predicts that absorption of light occurs preferably with increase of angular momentum. We generalize Fano's propensity rule to laser-assisted photoionization, consisting of absorption of an extreme-ultraviolet photon followed by absorption or emission of an infrared photon. The predicted asymmetry between absorption and emission leads to incomplete quantum interference in attosecond photoelectron interferometry. It explains both the angular dependence of the photoionization time delays and the delay dependence of the photoelectron angular distributions. Our theory is verified by experimental results in Ar in the 20-40 eV range.
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| 4. |
- Busto, David, et al.
(författare)
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Probing electronic decoherence with high-resolution attosecond photoelectron interferometry
- 2022
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Ingår i: European Physical Journal D. - : Springer Science and Business Media LLC. - 1434-6060 .- 1434-6079. ; 76:7
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Tidskriftsartikel (refereegranskat)abstract
- Abstract: Quantum coherence plays a fundamental role in the study and control of ultrafast dynamics in matter. In the case of photoionization, entanglement of the photoelectron with the ion is a well-known source of decoherence when only one of the particles is measured. Here, we investigate decoherence due to entanglement of the radial and angular degrees of freedom of the photoelectron. We study two-photon ionization via the 2s2p autoionizing state in He using high spectral resolution photoelectron interferometry. Combining experiment and theory, we show that the strong dipole coupling of the 2s2p and 2p2 states results in the entanglement of the angular and radial degrees of freedom. This translates, in angle-integrated measurements, into a dynamic loss of coherence during autoionization. Graphic Abstract: [Figure not available: see fulltext.]. © 2022, The Author(s).
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| 5. |
- Cheng, Yu Chen, et al.
(författare)
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Controlling photoionization using attosecond time-slit interferences
- 2020
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424. ; 117:20, s. 10727-10732
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Tidskriftsartikel (refereegranskat)abstract
- When small quantum systems, atoms or molecules, absorb a high-energy photon, electrons are emitted with a well-defined energy and a highly symmetric angular distribution, ruled by energy quantization and parity conservation. These rules are based on approximations and symmetries which may break down when atoms are exposed to ultrashort and intense optical pulses. This raises the question of their universality for the simplest case of the photoelectric effect. Here we investigate photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared laser field. We continuously control the energy of the photoelectrons and introduce an asymmetry in their emission direction, at variance with the idealized rules mentioned above. This control, made possible by the extreme temporal confinement of the light-matter interaction, opens a road in attosecond science, namely, the manipulation of ultrafast processes with a tailored sequence of attosecond pulses.
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| 6. |
- Kushawaha, Rajesh K., et al.
(författare)
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Multi-slit-type interference in carbon 2s photoionization of polyatomic molecules : from a fundamental effect to structural parameters
- 2019
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : ROYAL SOC CHEMISTRY. - 1463-9076 .- 1463-9084. ; 21:25, s. 13600-13610
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Tidskriftsartikel (refereegranskat)abstract
- In molecular photoemission, the analogue of the celebrated Young's double slit experiment is coherent electron emission from two equivalent atomic centers, giving rise to an interference pattern. Here multi-slit interference is investigated in inner-valence photoionization of propane, n-butane, isobutane and methyl peroxide. A more complex pattern is observed due to molecular orbital delocalization in polyatomic molecules, blurring the distinction between interference and diffraction. The potential to extract geometrical information is emphasized, as a more powerful extension of the EXAFS technique. Accurate reproduction of experimental features is obtained by simulations at the static Density Functional Theory level.
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| 7. |
- Mikaelsson, Sara, et al.
(författare)
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A high-repetition rate attosecond light source for time-resolved coincidence spectroscopy
- 2020
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Ingår i: Nanophotonics. - : Walter de Gruyter GmbH. - 2192-8614 .- 2192-8606. ; 10:1, s. 117-128
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Tidskriftsartikel (refereegranskat)abstract
- Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, subfemtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments, where several reaction products must be detected in coincidence, and for surface science applications where space charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high-repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses. We also present the first coincidence measurement of single-photon double-ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons.
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| 8. |
- Mikaelsson, Sara, et al.
(författare)
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A high-repetition rate attosecond light source for time-resolved coincidence spectroscopy
- 2021
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Ingår i: Frontiers in Optics and Photonics. - : De Gruyter. - 9783110710687 - 9783110709735 ; , s. 119-130
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Bokkapitel (refereegranskat)abstract
- Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, subfemtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments, where several reaction products must be detected in coincidence, and for surface science applications where space charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high-repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses. We also present the first coincidence measurement of single-photon dou-ble-ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons.
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| 9. |
- Mikaelsson, Sara, et al.
(författare)
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Controlled asymmetric photoelectron emission using electron wavepacket interference
- 2019
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Ingår i: 2019 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2019. - 9781728104690
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Konferensbidrag (refereegranskat)abstract
- Two-color ionization is a powerful method for characterizing light fields and investigating atomic and molecular physics with attosecond sources based on High Harmonic Generation (HHG). Depending on the time duration of the light fields, two main techniques have been established: streaking [1], appropriate in the regime where a single attosecond pulse is generated, and RABBIT, used instead when a relatively long fundamental pulse generates an XUV pulse train and the variation between consecutive XUV pulses is negligible [2]. In the regime where high harmonics are generated by a few-cycle fundamental pulse, however, both the amplitude and phase of the few resulting XUV pulses vary significantly, and this variation can be controlled by the CEP of the driving IR field [3]. In this work, we use attosecond pulse trains produced by HHG in argon using a 200 kHz-repetition rate, Carrier-Envelope-Phase (CEP) stable, 6-fs OPCPA laser system [4] and detect emitted photoelectrons from helium byby a three-dimensional (3D) momentum spectrometer [5]. With our excitation scheme, where a weak replica of the generating IR is overlapped with the short XUV pulse train for photoionization, we investigate the regime between the two limits represented by streaking and RABBIT.
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| 10. |
- Myhre, Rolf H., et al.
(författare)
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A theoretical and experimental benchmark study of core-excited states in nitrogen
- 2018
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 148:6
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Tidskriftsartikel (refereegranskat)abstract
- The high resolution near edge X-ray absorption fine structure spectrum of nitrogen displays the vibrational structure of the core-excited states. This makes nitrogen well suited for assessing the accuracy of different electronic structure methods for core excitations. We report high resolution experimental measurements performed at the SOLEIL synchrotron facility. These are compared with theoretical spectra calculated using coupled cluster theory and algebraic diagrammatic construction theory. The coupled cluster singles and doubles with perturbative triples model known as CC3 is shown to accurately reproduce the experimental excitation energies as well as the spacing of the vibrational transitions. The computational results are also shown to be systematically improved within the coupled cluster hierarchy, with the coupled cluster singles, doubles, triples, and quadruples method faithfully reproducing the experimental vibrational structure.
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