| 1. |
- Arnold, Cord L., et al.
(författare)
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Spatiotemporal coupling of attosecond pulses
- 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 ; Part F140-CLEO_Europe 2019
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Konferensbidrag (refereegranskat)abstract
- Attosecond pulses in the extreme ultraviolet (XUV) spectral range are today routinely generated via high-order harmonic generation (HHG), when intense ultrashort laser pulses are focused into a gaseous generation medium. The effect is most easily understood in a semi-classical picture [1]. An electron can tunnel ionize from the distorted atomic potential, pick up kinetic energy in the laser field, potentially return to its parent ion and recombine. The excess energy is emitted as XUV photon. The process repeats for every half-cycle of the driving field, resulting in a train of attosecond pulses and in the frequency domain in the well-known, odd-order comb of harmonics. Two main families of electron trajectories leading to the same photon energy can be distinguished into 'short' and 'long', according to their time of travel in the continuum. Due to the complicated nature of the HHG process, attosecond pulses usually cannot be separated into their temporal and spatial profiles, but instead have strong chromatic aberration and are spatio-temporally coupled [2-4].
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| 2. |
- Bertolino, Mattias, et al.
(författare)
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Thomas-Reiche-Kuhn correction for truncated configuration-interaction spaces : Case of laser-assisted dynamical interference
- 2022
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 106:4
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Tidskriftsartikel (refereegranskat)abstract
- The Thomas-Reiche-Kuhn sum rule is used to form an effective potential that is added to the time-dependent configuration-interaction singles (TDCIS) equations of motion in velocity gauge. The purpose of the effective potential is to include virtual coupling from singles to doubles, which is required for size-consistent velocity-gauge TDCIS results. The proposed method is compared to length-gauge TDCIS results for laser-assisted photoionization. Finally, a dynamical interference effect controlled by two-color fields is predicted for atomic targets.
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| 3. |
- Coudert-Alteirac, Hélène, et al.
(författare)
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Micro-focusing of broadband high-order harmonic radiation by a double toroidal mirror
- 2017
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Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 7:11
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Tidskriftsartikel (refereegranskat)abstract
- We present an optical system based on two toroidal mirrors in aWolter configuration to focus broadband extreme ultraviolet (XUV) radiation. Optimization of the focusing optics alignment is carried out with the aid of an XUV wavefront sensor. Back-propagation of the optimized wavefront to the focus yields a focal spot of 3.6 × 4.0 μm2 full width at half maximum, which is consistent with ray-tracing simulations that predict a minimum size of 3.0 × 3.2 μm2. This work is important for optimizing the intensity of focused high-order harmonics in order to reach the nonlinear interaction regime.
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| 4. |
- Dacasa, Hugo, et al.
(författare)
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Single-shot extreme-ultraviolet wavefront measurements of high-order harmonics
- 2019
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Ingår i: Optics Express. - 1094-4087. ; 27:3, s. 2656-2670
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Tidskriftsartikel (refereegranskat)abstract
- We perform wavefront measurements of high-order harmonics using an extreme-ultraviolet (XUV) Hartmann sensor and study how their spatial properties vary with different generation parameters, such as pressure in the nonlinear medium, fundamental pulse energy and duration as well as beam size. In some conditions, excellent wavefront quality (up to 휆/11) was obtained. The high throughput of the intense XUV beamline at the Lund Laser Centre allows us to perform single-shot measurements of both the full harmonic beam generated in argon and individual harmonics selected by multilayer mirrors. We theoretically analyze the relationship between the spatial properties of the fundamental and those of the generated high-order harmonics, thus gaining insight into the fundamental mechanisms involved in high-order harmonic generation (HHG).
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| 5. |
- Forbes, Ruaridh, et al.
(författare)
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Time-resolved site-selective imaging of predissociation and charge transfer dynamics : The CH3I B-band
- 2020
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 53:22
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Tidskriftsartikel (refereegranskat)abstract
- The predissociation dynamics of the 6s (B2E) Rydberg state of gas-phase CH3I were investigated by time-resolved Coulomb-explosion imaging using extreme ultraviolet (XUV) free-electron laser pulses. Inner-shell ionization at the iodine 4d edge was utilized to provide a site-specific probe of the ensuing dynamics. The combination of a velocity-map imaging (VMI) spectrometer coupled with the pixel imaging mass spectrometry (PImMS) camera permitted three-dimensional ionic fragment momenta to be recorded simultaneously for a wide range of iodine charge states. In accord with previous studies, initial excitation at 201.2 nm results in internal conversion and subsequent dissociation on the lower-lying A-state surface on a picosecond time scale. Examination of the time-dependent yield of low kinetic energy iodine fragments yields mechanistic insights into the predissociation and subsequent charge transfer following multiple ionization of the iodine products. The effect of charge transfer was observed through differing delay-dependencies of the various iodine charge states, from which critical internuclear distances for charge transfer could be inferred and compared to a classical over-the-barrier model. Time-dependent photofragment angular anisotropy parameters were extracted from the central slice of the Newton sphere, without Abel inversion, and highlight the effect of rotation of the parent molecule before dissociation, as observed in previous
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| 6. |
- 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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| 7. |
- 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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| 8. |
- Hoflund, Maria, et al.
(författare)
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Focusing Properties of High-Order Harmonics
- 2021
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Ingår i: Ultrafast Science. - : American Association for the Advancement of Science (AAAS). - 2765-8791. ; 2021
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Tidskriftsartikel (refereegranskat)abstract
- Many applications of the extreme ultraviolet (XUV) radiation obtained by high-order harmonic generation (HHG) in gases require a small focus area in order to enable attosecond pulses to reach a high intensity. Here, high-order harmonics generated in Ar with a multiterawatt laser system in a loose focusing geometry are focused to a few micrometers using two toroidal mirrors in a Wolter configuration with a high demagnification factor. Using a knife-edge measurement technique, we determine the position and size of the XUV foci as a function of harmonic order. We show that the focus properties vary with harmonic order and the generation conditions. Simulations, based on a classical description of the harmonic dipole phase and assuming that the individual harmonics can be described as Gaussian beams, reproduce the experimental behavior. We discuss how the generation geometry affects the intensity and duration of the focused attosecond pulses
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| 9. |
- Lee, Jason W.l., et al.
(författare)
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The Kinetic Energy of PAH Dication and Trication Dissociation Determined by Recoil-Frame Covariance Map Imaging
- 2022
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Ingår i: Physical Chemistry Chemical Physics. - 1463-9084. ; 24:38, s. 23096-23105
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Tidskriftsartikel (refereegranskat)abstract
- We investigated the dissociation of dications and trications of three polycyclic aromatic hydrocarbons (PAHs), fluorene, phenanthrene, and pyrene. PAHs are a family of molecules ubiquitous in space and involved in much of the chemistry of the interstellar medium. In our experiments, ions are formed by interaction with 30.3 nm extreme ultraviolet (XUV) photons, and their velocity map images are recorded using a PImMS2 multi-mass imaging sensor. Application of recoil-frame covariance analysis allows the total kinetic energy release (TKER) associated with multiple fragmentation channels to be determined to high precision, ranging 1.94-2.60 eV and 2.95-5.29 eV for the dications and trications, respectively. Experimental measurements are supported by Born-Oppenheimer molecular dynamics (BOMD) simulations.
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| 10. |
- Maclot, Sylvain, et al.
(författare)
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Dissociation dynamics of the diamondoid adamantane upon photoionization by XUV femtosecond pulses
- 2020
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Ingår i: Scientific Reports. - : Nature Research. - 2045-2322. ; 10:1
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Tidskriftsartikel (refereegranskat)abstract
- This work presents a photodissociation study of the diamondoid adamantane using extreme ultraviolet femtosecond pulses. The fragmentation dynamics of the dication is unraveled by the use of advanced ion and electron spectroscopy giving access to the dissociation channels as well as their energetics. To get insight into the fragmentation dynamics, we use a theoretical approach combining potential energy surface determination, statistical fragmentation methods and molecular dynamics simulations. We demonstrate that the dissociation dynamics of adamantane dications takes place in a two-step process: barrierless cage opening followed by Coulomb repulsion-driven fragmentation.
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