| 1. |
- Arnold, Cord L., et al.
(författare)
-
Spatiotemporal coupling of attosecond pulses
- 2019
-
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
-
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].
|
|
| 2. |
- Banerjee, Ambar, et al.
(författare)
-
Photoinduced bond oscillations in ironpentacarbonyl give delayed synchronous bursts of carbonmonoxide release
- 2022
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 13:1
-
Tidskriftsartikel (refereegranskat)abstract
- Early excited state dynamics in the photodissociation of transition metal carbonyls determines the chemical nature of short-lived catalytically active reaction intermediates. However, time-resolved experiments have not yet revealed mechanistic details in the sub-picosecond regime. Hence, in this study the photoexcitation of ironpentacarbonyl Fe(CO)5 is simulated with semi-classical excited state molecular dynamics. We find that the bright metal-to-ligand charge-transfer (MLCT) transition induces synchronous Fe-C oscillations in the trigonal bipyramidal complex leading to periodically reoccurring release of predominantly axial CO. Metaphorically the photoactivated Fe(CO)5 acts as a CO geyser, as a result of dynamics in the potential energy landscape of the axial Fe-C distances and non-adiabatic transitions between manifolds of bound MLCT and dissociative metal-centered (MC) excited states. The predominant release of axial CO ligands and delayed release of equatorial CO ligands are explained in a unified mechanism based on the σ*(Fe-C) anti-bonding character of the receiving orbital in the dissociative MC states.
|
|
| 3. |
- Berholts, Marta, et al.
(författare)
-
Quantum watch and its intrinsic proof of accuracy
- 2022
-
Ingår i: Physical Review Research. - : American Physical Society. - 2643-1564. ; 4:4
-
Tidskriftsartikel (refereegranskat)abstract
- We have investigated the rich dynamics of complex wave packets composed of multiple high-lying Rydbergstates in He. A quantitative agreement is found between theory and time-resolved photoelectron spectroscopyexperiments. We show that the intricate time dependence of such wave packets can be used for investigatingquantum defects and performing artifact-free timekeeping. The latter relies on the unique fingerprint that iscreated by the time-dependent photoionization of these complex wave packets. These fingerprints determinehow much time has passed since the wave packet was formed and provide an assurance that the measured time iscorrect. Unlike any other clock, this quantum watch does not utilize a counter and is fully quantum mechanicalin its nature. The quantum watch has the potential to become an invaluable tool in pump-probe spectroscopy dueto its simplicity, assurance of accuracy, and ability to provide an absolute timestamp, i.e., there is no need to findtime zero.
|
|
| 4. |
- Coudert-Alteirac, Hélène, et al.
(författare)
-
Micro-focusing of broadband high-order harmonic radiation by a double toroidal mirror
- 2017
-
Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 7:11
-
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.
|
|
| 5. |
- Dacasa, Hugo, et al.
(författare)
-
Single-shot extreme-ultraviolet wavefront measurements of high-order harmonics
- 2019
-
Ingår i: Optics Express. - 1094-4087. ; 27:3, s. 2656-2670
-
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).
|
|
| 6. |
- Hoflund, Maria, et al.
(författare)
-
Focusing Properties of High-Order Harmonics
- 2021
-
Ingår i: Ultrafast Science. - : American Association for the Advancement of Science (AAAS). - 2765-8791. ; 2021
-
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
|
|
| 7. |
- Jay, Raphael M., et al.
(författare)
-
Photochemical Formation and Electronic Structure of an Alkane ?-Complex from Time-Resolved Optical and X-ray Absorption Spectroscopy
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- C-H bond activation reactions with transition metals typically proceed via the formation of alkane ?-complexes, where an alkane C-H ?-bond binds to the metal. Due to the weak nature of metal-alkane bonds, ?-complexes are challenging to characterize experimentally. Here, we photochemically prepare the model ?-complex Cr(CO)5-alkane from Cr(CO)6 in octane solution and characterize the nature of its metal-ligand bonding interactions. Using femtosecond optical absorption spectroscopy, we find photo-induced CO dissociation from Cr(CO)6 to occur within the 100 fs time-resolution of the experiment. Rapid geminate recombination by a fraction of molecules is found to occur with a time constant of 150 fs. The formation of bare Cr(CO)5 in its singlet ground state is followed by complexation of an octane molecule from solution with a time constant of 8.2 ps. Picosecond X-ray absorption spectroscopy at the Cr L-edge and O K-edge provides unique information on the electronic structure of the Cr(CO)5-alkane ?-complex both from the metal and ligand perspectives. We find substantial destabilization of the lowest unoccupied molecular orbital upon coordination of the C-H bond to the undercoordinated Cr center in the Cr(CO)5-alkane ?-complex, accompanied with rehybridization between metal and ligand orbitals. Our study demonstrates the value of combining optical and X-ray spectroscopic methods as complementary tools to study the properties of alkane ?-complexes as the decisive intermediates in C-H bond activation reactions.
|
|
| 8. |
- Jay, Raphael M., et al.
(författare)
-
Photochemical Formation and Electronic Structure of an Alkane σ-Complex from Time-Resolved Optical and X-ray Absorption Spectroscopy
- 2024
-
Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 146:20, s. 14000-14011
-
Tidskriftsartikel (refereegranskat)abstract
- C–H bond activation reactions with transition metals typically proceed via the formation of alkane σ-complexes, where an alkane C–H σ-bond binds to the metal. Due to the weak nature of metal–alkane bonds, σ-complexes are challenging to characterize experimentally. Here, we establish the complete pathways of photochemical formation of the model σ-complex Cr(CO)5-alkane from Cr(CO)6 in octane solution and characterize the nature of its metal–ligand bonding interactions. Using femtosecond optical absorption spectroscopy, we find photoinduced CO dissociation from Cr(CO)6 to occur within the 100 fs time resolution of the experiment. Rapid geminate recombination by a fraction of molecules is found to occur with a time constant of 150 fs. The formation of bare Cr(CO)5 in its singlet ground state is followed by complexation of an octane molecule from solution with a time constant of 8.2 ps. Picosecond X-ray absorption spectroscopy at the Cr L-edge and O K-edge provides unique information on the electronic structure of the Cr(CO)5-alkane σ-complex from both the metal and ligand perspectives. Based on clear experimental observables, we find substantial destabilization of the lowest unoccupied molecular orbital upon coordination of the C–H bond to the undercoordinated Cr center in the Cr(CO)5-alkane σ-complex, and we define this as a general, orbital-based descriptor of the metal–alkane bond. Our study demonstrates the value of combining optical and X-ray spectroscopic methods as complementary tools to study the stability and reactivity of alkane σ-complexes in their role as the decisive intermediates in C–H bond activation reactions.
|
|
| 9. |
- Jay, Raphael, et al.
(författare)
-
Tracking C–H activation with orbital resolution
- 2023
-
Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 380:6648, s. 955-960
-
Tidskriftsartikel (refereegranskat)abstract
- Transition metal reactivity toward carbon-hydrogen (C-H) bonds hinges on the interplay of electron donation and withdrawal at the metal center. Manipulating this reactivity in a controlled way is difficult because the hypothesized metal-alkane charge-transfer interactions are challenging to access experimentally. Using time-resolved x-ray spectroscopy, we track the charge-transfer interactions during C-H activation of octane by a cyclopentadienyl rhodium carbonyl complex. Changes in oxidation state as well as valence-orbital energies and character emerge in the data on a femtosecond to nanosecond timescale. The x-ray spectroscopic signatures reflect how alkane-to-metal donation determines metal-alkane complex stability and how metal-to-alkane back-donation facilitates C-H bond cleavage by oxidative addition. The ability to dissect charge-transfer interactions on an orbital level provides opportunities for manipulating C-H reactivity at transition metals.
|
|
| 10. |
- Kühn, Sergei, et al.
(författare)
-
The ELI-ALPS facility : The next generation of attosecond sources
- 2017
-
Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 50:13
-
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.
|
|
| 11. |
- Maclot, Sylvain, et al.
(författare)
-
Dissociation dynamics of the diamondoid adamantane upon photoionization by XUV femtosecond pulses
- 2020
-
Ingår i: Scientific Reports. - : Nature Research. - 2045-2322. ; 10:1
-
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.
|
|
| 12. |
- Malm, Erik, et al.
(författare)
-
Singleshot polychromatic coherent diffractive imaging with a high-order harmonic source
- 2020
-
Ingår i: Optics Express. - 1094-4087. ; 28:1, s. 394-404
-
Tidskriftsartikel (refereegranskat)abstract
- Singleshot polychromatic coherent diffractive imaging is performed with a high-intensity high-order harmonic generation source. The coherence properties are analyzed and several reconstructions show the shot-to-shot fluctuations of the incident beam wavefront. The method is based on a multi-step approach. First, the spectrum is extracted from double-slit diffraction data. The spectrum is used as input to extract the monochromatic sample diffraction pattern, then phase retrieval is performed on the quasi-monochromatic data to obtain the sample's exit surface wave. Reconstructions based on guided error reduction (ER) and alternating direction method of multipliers (ADMM) are compared. ADMM allows additional penalty terms to be included in the cost functional to promote sparsity within the reconstruction.
|
|
| 13. |
- Peschel, Jasper, et al.
(författare)
-
Attosecond dynamics of multi-channel single photon ionization
- 2022
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 13:1
-
Tidskriftsartikel (refereegranskat)abstract
- Photoionization of atoms and molecules is one of the fastest processes in nature. The understanding of the ultrafast temporal dynamics of this process often requires the characterization of the different angular momentum channels over a broad energy range. Using a two-photon interferometry technique based on extreme ultraviolet and infrared ultrashort pulses, we measure the phase and amplitude of the individual angular momentum channels as a function of kinetic energy in the outer-shell photoionization of neon. This allows us to unravel the influence of channel interference as well as the effect of the short-range, Coulomb and centrifugal potentials, on the dynamics of the photoionization process.
|
|
| 14. |
- Rading, Linnea, et al.
(författare)
-
A versatile velocity map ion-electron covariance imaging spectrometer for high-intensity XUV experiments
- 2018
-
Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 8:6
-
Tidskriftsartikel (refereegranskat)abstract
- We report on the design and performance of a velocity map imaging (VMI) spectrometer optimized for experiments using high-intensity extreme ultraviolet (XUV) sources such as laser-driven high-order harmonic generation (HHG) sources and free-electron lasers (FELs). Typically exhibiting low repetition rates and high single-shot count rates, such experiments do not easily lend themselves to coincident detection of photo-electrons and -ions. In order to obtain molecular frame or reaction channel-specific information, one has to rely on other correlation techniques, such as covariant detection schemes. Our device allows for combining different photo-electron and -ion detection modes for covariance analysis. We present the expected performance in the different detection modes and present the first results using an intense high-order harmonic generation (HHG) source.
|
|
| 15. |
- Wikmark, Hampus
(författare)
-
Spatial and temporal aspects of intense attosecond pulses for pump-probe experiments
- 2019
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Nuclear and electronic dynamics in atoms and molecules are the foundation of many physical processes and chemical reactions. Often, these dynamics take place on timescales so much shorter than those commonly encountered that they are called ultrafast. In order to study ultrafast phenomena, time-resolved techniques such as pump-probe experiments, involving ultrafast light pulses, are necessary. For these experiments to be successful, the properties of ultrafast light pulses must be carefully controlled and examined in order to discern their influence on the experiment. This thesis deals with the spatial and temporal properties of XUV light, generated through the process of high-order harmonic generation in gases, using an intense IR laser beam. The influence of the spatial properties of this generating laser on the XUV has been studied, as has the influence of the XUV light's spatial properties on its focusability and peak intensity. The generated high-order harmonics are also used to study physical phenomena such as multiphoton ionization, something that requires high intensities. An instrument for simultaneous studies of ions and electrons produced by photoionization is also presented. The efforts towards ultrafast pump-probe experiments include designs for interferometer setups to enable these experiments. Some preliminary results of interferometer testing are also given, including a proof of principle of XUV-IR pump-probe experiments on the Lund Laser Centre intense XUV beamline.
|
|
| 16. |
- Wikmark, Hampus, et al.
(författare)
-
Spatiotemporal coupling of attosecond pulses
- 2019
-
Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424. ; 116:11, s. 4779-4787
-
Tidskriftsartikel (refereegranskat)abstract
- The shortest light pulses produced to date are of the order of a few tens of attoseconds, with central frequencies in the extreme UV range and bandwidths exceeding tens of electronvolts. They are often produced as a train of pulses separated by half the driving laser period, leading in the frequency domain to a spectrum of high, odd-order harmonics. As light pulses become shorter and more spectrally wide, the widely used approximation consisting of writing the optical waveform as a product of temporal and spatial amplitudes does not apply anymore. Here, we investigate the interplay of temporal and spatial properties of attosecond pulses. We show that the divergence and focus position of the generated harmonics often strongly depend on their frequency, leading to strong chromatic aberrations of the broadband attosecond pulses. Our argument uses a simple analytical model based on Gaussian optics, numerical propagation calculations, and experimental harmonic divergence measurements. This effect needs to be considered for future applications requiring highquality focusing while retaining the broadband/ultrashort characteristics of the radiation.
|
|
