| 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.
|
|
