1. |
- Stern, S., et al.
(författare)
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Toward atomic resolution diffractive imaging of isolated molecules with X-ray free-electron lasers
- 2014
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Ingår i: Faraday Discussions. - : Royal Society of Chemistry (RSC). - 1364-5498. ; 171, s. 393-418
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Tidskriftsartikel (refereegranskat)abstract
- We give a detailed account of the theoretical analysis and the experimental results of an X-ray-diffraction experiment on quantum-state selected and strongly laser-aligned gasphase ensembles of the prototypical large asymmetric rotor molecule 2,5-diiodobenzonitrile, performed at the Linac Coherent Light Source [Phys. Rev. Lett. 112, 083002 (2014)]. This experiment is the first step toward coherent diffractive imaging of structures and structural dynamics of isolated molecules at atomic resolution, i.e., picometers and femtoseconds, using X-ray free-electron lasers.
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2. |
- Arnold, C. L., et al.
(författare)
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The ELI-ALPS secondary sources : A getaway to scientific excellence
- 2013
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Ingår i: 2013 Conference on Lasers and Electro-Optics, CLEO 2013. - 9781557529725 ; 2013
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Konferensbidrag (refereegranskat)abstract
- The essence of ELI-ALPS, the laser driven secondary sources ranging from X-ray and X-UV to THz with duration as short as tens of attoseconds, are designed to be available for users from 2016.
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3. |
- Gryzlova, E. V., et al.
(författare)
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Doubly resonant three-photon double ionization of Ar atoms induced by an EUV free-electron laser
- 2011
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 84:6
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Tidskriftsartikel (refereegranskat)abstract
- A mechanism for three-photon double ionization of atoms by extreme-ultraviolet free-electron laser pulses is revealed, where in a sequential process the second ionization step, proceeding via resonant two-photon ionization of ions, is strongly enhanced by the excitation of ionic autoionizing states. In contrast to the conventional model, the mechanism explains the observed relative intensities of photoelectron peaks and their angular dependence in three-photon double ionization of argon.
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4. |
- Rolles, D., et al.
(författare)
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Femtosecond x-ray photoelectron diffraction on gas-phase dibromobenzene molecules
- 2014
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 47:12
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Tidskriftsartikel (refereegranskat)abstract
- We present time-resolved femtosecond photoelectron momentum images and angular distributions of dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules measured in a near-infrared pump, soft-x-ray probe experiment performed at an x-ray free-electron laser. The observed alignment dependence of the bromine 2p photoelectron angular distributions is compared to density functional theory calculations and interpreted in terms of photoelectron diffraction. While no clear time-dependent effects are observed in the angular distribution of the Br(2p) photoelectrons, other, low-energy electrons show a pronounced dependence on the time delay between the near-infrared laser and the x-ray pulse.
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5. |
- Duesterer, S., et al.
(författare)
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Interference in the angular distribution of photoelectrons in superimposed XUV and optical laser fields
- 2013
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16
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Tidskriftsartikel (refereegranskat)abstract
- The angular distribution of photoelectrons ejected during the ionization of Ne atoms by extreme ultraviolet (XUV) free-electron laser radiation in the presence of an intense near infrared (NIR) dressing field was investigated experimentally and theoretically. A highly nonlinear process with absorption and emission of more than ten NIR photons results in the formation of numerous sidebands. The amplitude of the sidebands varies strongly with the emission angle and the angular distribution pattern reveals clear signatures of interferences between the different angular momenta for the outgoing electron in the multi-photon process. As a specific feature, the central photoelectron line is characterized at the highest NIR fields by an angular distribution, which is peaked perpendicularly to both the XUV and NIR polarization directions. Experimental results are reproduced by a theoretical model based on the strong field approximation.
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6. |
- Mondal, S., et al.
(författare)
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Photoelectron angular distributions for the two-photon sequential double ionization of xenon by ultrashort extreme ultraviolet free electron laser pulses
- 2013
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16
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Tidskriftsartikel (refereegranskat)abstract
- Xenon atoms are double-ionized by sequential two-photon absorption by ultrashort extreme ultraviolet free-electron laser pulses with a photon energy of 23.0 and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The angular distributions of photoelectrons generated by two-photon double ionization are obtained using velocity map imaging. The results are reproduced reasonably well by the present theoretical calculations within the multi-configurational Dirac-Fock approach.
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7. |
- Pathak, S., et al.
(författare)
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Tracking the ultraviolet-induced photochemistry of thiophenone during and after ultrafast ring opening
- 2020
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Ingår i: Nature Chemistry. - : Springer Science and Business Media LLC. - 1755-4330 .- 1755-4349. ; 12:9, s. 795-800
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Tidskriftsartikel (refereegranskat)abstract
- Photoinduced isomerization reactions lie at the heart of many chemical processes in nature. The mechanisms of such reactions are determined by a delicate interplay of coupled electronic and nuclear dynamics occurring on the femtosecond scale, followed by the slower redistribution of energy into different vibrational degrees of freedom. Here we apply time-resolved photoelectron spectroscopy with a seeded extreme ultraviolet free-electron laser to trace the ultrafast ring opening of gas-phase thiophenone molecules following ultraviolet photoexcitation. When combined with ab initio electronic structure and molecular dynamics calculations of the excited- and ground-state molecules, the results provide insights into both the electronic and nuclear dynamics of this fundamental class of reactions. The initial ring opening and non-adiabatic coupling to the electronic ground state are shown to be driven by ballistic S-C bond extension and to be complete within 350 fs. Theory and experiment also enable visualization of the rich ground-state dynamics that involve the formation of, and interconversion between, ring-opened isomers and the cyclic structure, as well as fragmentation over much longer timescales.
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8. |
- Rouzee, A., et al.
(författare)
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Angle-resolved photoelectron spectroscopy of sequential three-photon triple ionization of neon at 90.5 eV photon energy
- 2011
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 83:3
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Tidskriftsartikel (refereegranskat)abstract
- Multiple photoionization of neon atoms by a strong 13.7 nm (90.5 eV) laser pulse has been studied at the FLASH free electron laser in Hamburg. A velocity map imaging spectrometer was used to record angle-resolved photoelectron spectra on a single-shot basis. Analysis of the evolution of the spectra with the FEL pulse energy in combination with extensive theoretical calculations allows the ionization pathways that contribute to be assigned, revealing the occurrence of sequential three-photon triple ionization.
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9. |
- Rouzee, A., et al.
(författare)
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Towards imaging of ultrafast molecular dynamics using FELs
- 2013
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16
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Tidskriftsartikel (refereegranskat)abstract
- The dissociation dynamics induced by a 100 fs, 400 nm laser pulse in a rotationally cold Br-2 sample was characterized by Coulomb explosion imaging (CEI) using a time-delayed extreme ultra-violet (XUV) FEL pulse, obtained from the Free electron LASer in Hamburg (FLASH). The momentum distribution of atomic fragments resulting from the 400 nm-induced dissociation was measured with a velocity map imaging spectrometer and used to monitor the internuclear distance as the molecule dissociated. By employing the simultaneously recorded in-house timing electro-optical sampling data, the time resolution of the final results could be improved to 300 fs, compared to the inherent 500 fs time-jitter of the FEL pulse. Before dissociation, the Br-2 molecules were transiently 'fixed in space' using laser-induced alignment. In addition, similar alignment techniques were used on CO2 molecules to allow the measurement of the photoelectron angular distribution (PAD) directly in the molecular frame (MF). Our results on MFPADs in aligned CO2 molecules, together with our investigation of the dissociation dynamics of the Br-2 molecules with CEI, show that information about the evolving molecular structure and electronic geometry can be retrieved from such experiments, therefore paving the way towards the study of complex non-adiabatic dynamics in molecules through XUV time-resolved photoion and photoelectron spectroscopy.
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10. |
- Walmsley, T., et al.
(författare)
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Characterizing the multi-dimensional reaction dynamics of dihalomethanes using XUV-induced Coulomb explosion imaging
- 2023
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Ingår i: Journal of Chemical Physics. - 0021-9606. ; 159:14
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Tidskriftsartikel (refereegranskat)abstract
- Site-selective probing of iodine 4d orbitals at 13.1 nm was used to characterize the photolysis of CH2I2 and CH2BrI initiated at 202.5 nm. Time-dependent fragment ion momenta were recorded using Coulomb explosion imaging mass spectrometry and used to determine the structural dynamics of the dissociating molecules. Correlations between these fragment momenta, as well as the onset times of electron transfer reactions between them, indicate that each molecule can undergo neutral three-body photolysis. For CH2I2, the structural evolution of the neutral molecule was simultaneously characterized along the C-I and I-C-I coordinates, demonstrating the sensitivity of these measurements to nuclear motion along multiple degrees of freedom.
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11. |
- Johnsson, Per, et al.
(författare)
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Characterization of a two-color pump-probe setup at FLASH using a velocity map imaging spectrometer
- 2010
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Ingår i: Optics Letters. - 0146-9592. ; 35:24, s. 4163-4165
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Tidskriftsartikel (refereegranskat)abstract
- We report on the implementation of a high-count-rate charged particle imaging detector for two-color pump-probe experiments at the free electron laser in Hamburg (FLASH). In doing so, we have developed a procedure for finding the spatial and temporal overlap between the extreme UV free electron laser (FEL) pulses and the IR pulses, which allows for complete alignment of the setup in situations where the region of overlap between the FEL and the IR is not easily accessible by means of imaging optics. (C) 2010 Optical Society of America
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12. |
- Kornilov, O., et al.
(författare)
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Coulomb explosion of diatomic molecules in intense XUV fields mapped by partial covariance
- 2013
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 46:16
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Tidskriftsartikel (refereegranskat)abstract
- Single-shot time-of-flight spectra for Coulomb explosion of N-2 and I-2 molecules have been recorded at the Free Electron LASer in Hamburg (FLASH) and have been analysed using a partial covariance mapping technique. The partial covariance analysis unravels a detailed picture of all significant Coulomb explosion pathways, extending up to the N4+-N5+ channel for nitrogen and up to the I8+-I9+ channel for iodine. The observation of the latter channel is unexpected if only sequential ionization processes from the ground state ions are considered. The maximum kinetic energy release extracted from the covariance maps for each dissociation channel shows that Coulomb explosion of nitrogen molecules proceeds much faster than that of the iodine. The N-2 ionization dynamics is modelled using classical trajectory simulations in good agreement with the outcome of the experiments. The results suggest that covariance mapping of the Coulomb explosion can be used to measure the intensity and pulse duration of free-electron lasers.
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13. |
- Neidel, Ch, et al.
(författare)
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Probing Time-Dependent Molecular Dipoles on the Attosecond Time Scale
- 2013
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Ingår i: Physical Review Letters. - 1079-7114. ; 111:3
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Tidskriftsartikel (refereegranskat)abstract
- Photoinduced molecular processes start with the interaction of the instantaneous electric field of the incident light with the electronic degrees of freedom. This early attosecond electronic motion impacts the fate of the photoinduced reactions. We report the first observation of attosecond time scale electron dynamics in a series of small-and medium-sized neutral molecules (N-2, CO2, and C2H4), monitoring time-dependent variations of the parent molecular ion yield in the ionization by an attosecond pulse, and thereby probing the time-dependent dipole induced by a moderately strong near-infrared laser field. This approach can be generalized to other molecular species and may be regarded as a first example of molecular attosecond Stark spectroscopy.
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14. |
- Siu, W., et al.
(författare)
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Attosecond control of dissociative ionization of O(2) molecules
- 2011
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 84:6
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Tidskriftsartikel (refereegranskat)abstract
- We demonstrate that dissociative ionization of O(2) can be controlled by the relative delay between an attosecond pulse train (APT) and a copropagating infrared (IR) field. Our experiments reveal a dependence of both the branching ratios between a range of electronic states and the fragment angular distributions on the extreme ultraviolet (XUV) to IR time delay. The observations go beyond adiabatic propagation of dissociative wave packets on IR-induced quasistatic potential energy curves and are understood in terms of an IR-induced coupling between electronic states in the molecular ion.
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15. |
- Borne, Kurtis D., et al.
(författare)
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Ultrafast electronic relaxation pathways of the molecular photoswitch quadricyclane
- 2024
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Ingår i: NATURE CHEMISTRY. - : Springer Nature. - 1755-4330 .- 1755-4349. ; 16, s. 499-505
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Tidskriftsartikel (refereegranskat)abstract
- The light-induced ultrafast switching between molecular isomers norbornadiene and quadricyclane can reversibly store and release a substantial amount of chemical energy. Prior work observed signatures of ultrafast molecular dynamics in both isomers upon ultraviolet excitation but could not follow the electronic relaxation all the way back to the ground state experimentally. Here we study the electronic relaxation of quadricyclane after exciting in the ultraviolet (201 nanometres) using time-resolved gas-phase extreme ultraviolet photoelectron spectroscopy combined with non-adiabatic molecular dynamics simulations. We identify two competing pathways by which electronically excited quadricyclane molecules relax to the electronic ground state. The fast pathway (<100 femtoseconds) is distinguished by effective coupling to valence electronic states, while the slow pathway involves initial motions across Rydberg states and takes several hundred femtoseconds. Both pathways facilitate interconversion between the two isomers, albeit on different timescales, and we predict that the branching ratio of norbornadiene/quadricyclane products immediately after returning to the electronic ground state is approximately 3:2.
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16. |
- Kelkensberg, F., et al.
(författare)
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Attosecond Control in Photoionization of Hydrogen Molecules
- 2011
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Ingår i: Physical Review Letters. - 1079-7114. ; 107:4
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Tidskriftsartikel (refereegranskat)abstract
- We report experiments where hydrogen molecules were dissociatively ionized by an attosecond pulse train in the presence of a near-infrared field. Fragment ion yields from distinguishable ionization channels oscillate with a period that is half the optical cycle of the IR field. For molecules aligned parallel to the laser polarization axis, the oscillations are reproduced in two-electron quantum simulations, and can be explained in terms of an interference between ionization pathways that involve different harmonic orders and a laser-induced coupling between the 1s sigma(g) and 2p sigma(u) states of the molecular ion. This leads to a situation where the ionization probability is sensitive to the instantaneous polarization of the molecule by the IR electric field and demonstrates that we have probed the IR-induced electron dynamics with attosecond pulses.
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17. |
- Kelkensberg, F., et al.
(författare)
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XUV ionization of aligned molecules
- 2011
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Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 84:5, s. 051404-051404
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Tidskriftsartikel (refereegranskat)abstract
- New extreme-ultraviolet (XUV) light sources such as high-order-harmonic generation (HHG) and free-electron lasers (FELs), combined with laser-induced alignment techniques, enable novel methods for making molecular movies based on measuring molecular frame photoelectron angular distributions. Experiments are presented where CO2 molecules were impulsively aligned using a near-infrared laser and ionized using femtosecond XUV pulses obtained by HHG. Measured electron angular distributions reveal contributions from four orbitals and the onset of the influence of the molecular structure.
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18. |
- Kuepper, Jochen, et al.
(författare)
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X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
- 2014
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 112:8, s. 083002-
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Tidskriftsartikel (refereegranskat)abstract
- We report experimental results on x-ray diffraction of quantum-state-selected and strongly aligned ensembles of the prototypical asymmetric rotor molecule 2,5-diiodobenzonitrile using the Linac Coherent Light Source. The experiments demonstrate first steps toward a new approach to diffractive imaging of distinct structures of individual, isolated gas-phase molecules. We confirm several key ingredients of single molecule diffraction experiments: the abilities to detect and count individual scattered x-ray photons in single shot diffraction data, to deliver state-selected, e.g., structural-isomer-selected, ensembles of molecules to the x-ray interaction volume, and to strongly align the scattering molecules. Our approach, using ultrashort x-ray pulses, is suitable to study ultrafast dynamics of isolated molecules.
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19. |
- Schuette, B., et al.
(författare)
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Recombination-Induced Autoionization Process in Rare-Gas Clusters
- 2015
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Ingår i: Ultrafast Phenomena XIX. - Cham : Springer International Publishing. - 0930-8989. ; 162, s. 56-59
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Konferensbidrag (refereegranskat)abstract
- We investigate electron-ion recombination to excited states in atomic clusters exposed to intense NIR and XUV pulses, which leads to a yet undiscovered autoionization mechanism as a consequence of multiple recombination processes.
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20. |
- Schuette, B., et al.
(författare)
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Tracing Electron-Ion Recombination in Nanoplasmas Produced by Extreme-Ultraviolet Irradiation of Rare-Gas Clusters
- 2014
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Ingår i: Physical Review Letters. - 1079-7114. ; 112:25
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Tidskriftsartikel (refereegranskat)abstract
- We investigate electron-ion recombination in nanoplasmas produced by the ionization of rare-gas clusters with intense femtosecond extreme-ultraviolet (XUV) pulses. The relaxation dynamics following XUV irradiation is studied using time-delayed 790-nm pulses, revealing the generation of a large number of excited atoms resulting from electron-ion recombination. In medium-sized Ar-Xe clusters, these atoms are preferentially created in the Xe core within 10 ps after the cluster ionization. The ionization of excited atoms serves as a sensitive probe for monitoring the cluster expansion dynamics up to the ns time scale.
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