| 1. |
- Lever, Fabiano, et al.
(författare)
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Core-level spectroscopy of 2-thiouracil at the sulfur L1 and L2,3-edges utilizing a sase free-electron laser
- 2021
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Ingår i: Molecules. - : MDPI AG. - 1420-3049. ; 26:1
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Tidskriftsartikel (refereegranskat)abstract
- In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L1-and L2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster–Kronig and Auger– Meitner emission at the L1-and L2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.
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| 2. |
- Metje, Jan, et al.
(författare)
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URSA-PQ: A mobile and flexible pump-probe instrument for gas phase samples at the flash free electron laser
- 2020
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Ingår i: Applied Sciences (Switzerland). - : MDPI AG. - 2076-3417. ; 10, s. 1-13
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Tidskriftsartikel (refereegranskat)abstract
- We present a highly flexible and portable instrument to perform pump-probe spectroscopy with an optical and an X-ray pulse in the gas phase. The so-called URSA-PQ (German for ‘Ultraschnelle Röntgenspektroskopie zur Abfrage der Photoenergiekonversion an Quantensystemen’, Engl. ‘ultrafast X-ray spectroscopy for probing photoenergy conversion in quantum systems’) instrument is equipped with a magnetic bottle electron spectrometer (MBES) and tools to characterize the spatial and temporal overlap of optical and X-ray laser pulses. Its adherence to the CAMP instrument dimensions allows for a wide range of sample sources as well as other spectrometers to be included in the setup. We present the main design and technical features of the instrument. The MBES performance was evaluated using Kr M4,5NN Auger lines using backfilled Kr gas, with an energy resolution ΔE/E ≅ 1/40 in the integrating operative mode. The time resolution of the setup at FLASH 2 FL 24 has been characterized with the help of an experiment on 2-thiouracil that is inserted via the instruments’ capillary oven. We find a time resolution of 190 fs using the molecular 2p photoline shift and attribute this to different origins in the UV-pump—the X-ray probe setup.
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| 3. |
- 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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| 4. |
- Schäfer, Rudi, et al.
(författare)
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Credit risk - A structural model with jumps and correlations
- 2007
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Ingår i: Physica A: Statistical Mechanics and its Applications. - : Elsevier BV. - 0378-4371. ; 383:2, s. 533-569
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Tidskriftsartikel (refereegranskat)abstract
- We set up a structural model to study credit risk for a portfolio containing several or many credit contracts. The model is based on a jump-diffusion process for the risk factors, i.e. for the company assets. We also include correlations between the companies. We discuss that models of this type have much in common with other problems in statistical physics and in the theory of complex systems. We study a simplified version of our model analytically. Furthermore, we perform extensive numerical simulations for the full model. The observables are the loss distribution of the credit portfolio, its moments and other quantities derived thereof. We compile detailed information about the parameter dependence of these observables. In the course of setting up and analyzing our model, we also give a review of credit risk modeling for a physics audience. (c) 2007 Elsevier B.V. All rights reserved.
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| 5. |
- Wolf, Thomas J. A., et al.
(författare)
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Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra
- 2017
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Ingår i: Applied Sciences. - : MDPI AG. - 2076-3417 .- 1454-5101. ; 7:7
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Tidskriftsartikel (refereegranskat)abstract
- Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymines neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.
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| 6. |
- Young, Linda, et al.
(författare)
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Roadmap of ultrafast x-ray atomic and molecular physics
- 2018
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Ingår i: Journal of Physics B: Atomic, Molecular and Optical Physics. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 51:3
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Forskningsöversikt (refereegranskat)abstract
- X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm-2) of x-rays at wavelengths down to ∼1 Ångstrom, and HHG provides unprecedented time resolution (∼50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ∼280 eV (44 Ångstroms) and the bond length in methane of ∼1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.
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