@article{CollaborationAbramowskiAharonianetal.2014, author = {Collaboration, H. E. S. S. and Abramowski, Attila and Aharonian, Felix A. and Benkhali, Faical Ait and Akhperjanian, A. G. and Ang{\"u}ner, Ekrem Oǧuzhan and Anton, Gisela and Balenderan, Shangkari and Balzer, Arnim and Barnacka, Anna and Becherini, Yvonne and Tjus, J. Becker and Bernl{\"o}hr, K. and Birsin, E. and Bissaldi, E. and Biteau, Jonathan and Boettcher, Markus and Boisson, Catherine and Bolmont, J. and Bordas, Pol and Brucker, J. and Brun, Francois and Brun, Pierre and Bulik, Tomasz and Carrigan, Svenja and Casanova, Sabrina and Cerruti, M. and Chadwick, Paula M. and Chalme-Calvet, R. and Chaves, Ryan C. G. and Cheesebrough, A. and Chretien, M. and Colafrancesco, Sergio and Cologna, Gabriele and Conrad, Jan and Couturier, C. and Cui, Y. and Dalton, M. and Daniel, M. K. and Davids, I. D. and Degrange, B. and Deil, C. and de Wilt, P. and Dickinson, H. J. and Djannati-Ata{\"i}, A. and Domainko, W. and Dubus, G. and Dutson, K. and Dyks, J. and Dyrda, M. and Edwards, T. and Egberts, Kathrin and Eger, P. and Espigat, P. and Farnier, C. and Fegan, S. and Feinstein, F. and Fernandes, M. V. and Fernandez, D. and Fiasson, A. and Fontaine, G. and Foerster, A. and Fuessling, M. and Gajdus, M. and Gallant, Y. A. and Garrigoux, T. and Giavitto, G. and Giebels, B. and Glicenstein, J. F. and Grondin, M. -H. and Grudzinska, M. and Haeffner, S. and Hahn, J. and Harris, J. and Heinzelmann, G. and Henri, G. and Hermann, G. and Hervet, O. and Hillert, A. and Hinton, James Anthony and Hofmann, W. and Hofverberg, P. and Holler, M. and Horns, Dieter and Jacholkowska, A. and Jahn, C. and Jamrozy, M. and Janiak, M. and Jankowsky, F. and Jung, I. and Kastendieck, M. A. and Katarzynski, K. and Katz, U. and Kaufmann, S. and Khelifi, B. and Kieffer, M. and Klepser, S. and Klochkov, D. and Kluzniak, W. and Kneiske, T. and Kolitzus, D. and Komin, Nu. and Kosack, K. and Krakau, S. and Krayzel, F. and Krueger, P. P. and Laffon, H. and Lamanna, G. and Lefaucheur, J. and Lemiere, A. and Lemoine-Goumard, M. and Lenain, J. -P. and Lennarz, D. and Lohse, T. and Lopatin, A. and Lu, C. -C. and Marandon, V. and Marcowith, Alexandre and Marx, R. and Maurin, G. and Maxted, N. and Mayer, M. and McComb, T. J. L. and Mehault, J. and Meintjes, P. J. and Menzler, U. and Meyer, M. and Moderski, R. and Mohamed, M. and Moulin, Emmanuel and Murach, T. and Naumann, C. L. and de Naurois, M. and Niemiec, J. and Nolan, S. J. and Oakes, L. and Ohm, S. and Wilhelmi, E. de Ona and Opitz, B. and Ostrowski, M. and Oya, I. and Panter, M. and Parsons, R. D. and Arribas, M. Paz and Pekeur, N. W. and Pelletier, G. and Perez, J. and Petrucci, P. -O. and Peyaud, B. and Pita, S. and Poon, H. and Puehlhofer, G. and Punch, M. and Quirrenbach, A. and Raab, S. and Raue, M. and Reimer, A. and Reimer, O. and Renaud, M. and de los Reyes, R. and Rieger, F. and Rob, L. and Romoli, C. and Rosier-Lees, S. and Rowell, G. and Rudak, B. and Rulten, C. B. and Sahakian, V. and Sanchez, David M. and Santangelo, Andrea and Schlickeiser, R. and Schuessler, F. and Schulz, A. and Schwanke, U. and Schwarzburg, S. and Schwemmer, S. and Sol, H. and Spengler, G. and Spies, F. and Stawarz, L. and Steenkamp, R. and Stegmann, Christian and Stinzing, F. and Stycz, Kornelia and Sushch, Iurii and Szostek, A. and Tavernet, J. -P. and Tavernier, T. and Taylor, A. M. and Terrier, R. and Tluczykont, M. and Trichard, C. and Valerius, K. and van Eldik, C. and van Soelen, B. and Vasileiadis, G. and Venter, C. and Viana, A. and Vincent, P. and Voelk, H. J. and Volpe, F. and Vorster, M. and Vuillaume, T. and Wagner, S. J. and Wagner, P. and Ward, M. and Weidinger, M. and Weitzel, Q. and White, R. and Wierzcholska, A. and Willmann, P. and Woernlein, A. and Wouters, D. and Zabalza, V. and Zacharias, M. and Zajczyk, A. and Zdziarski, A. A. and Zech, Alraune and Zechlin, H. -S.}, title = {HESS observations of the Crab during its March 2013 GeV gamma-ray flare}, series = {Astronomy and astrophysics : an international weekly journal}, volume = {562}, journal = {Astronomy and astrophysics : an international weekly journal}, publisher = {EDP Sciences}, address = {Les Ulis}, issn = {0004-6361}, doi = {10.1051/0004-6361/201323013}, pages = {5}, year = {2014}, abstract = {Context. On March 4, 2013 the Fermi-EAT and AGILE reported a flare from the direction of the Crab nebula in which the high-energy (HE; E > 100 MeV) flux was six times above its quiescent level. Simultaneous observations in other energy bands give us hints about the emission processes during the flare episode and the physics of pulsar wind nebulae in general. Aims. We search for variability in the emission of the Crab nebula at very-high energies (VHF,; E > 100 GeV), using contemporaneous data taken with the H.E.S.S. array of Cherenkov telescopes. Methods. Observational data taken with the H.E.S.S. instrument on five consecutive days during the flare were analysed for the flux and spectral shape of the emission from the Crab nebula. Night-wise light curves are presented with energy thresholds of 1 TeV and 5 TeV. Results. The observations conducted with H.E.S.S. on March 6 to March 10, 2013 show no significant changes in the flux. They limit the variation in the integral flux above 1 TeV to less than 63\% and the integral flux above 5 TeV to less than 78\% at a 95\% confidence level.}, language = {en} } @article{LeverMayerMetjeetal.2021, author = {Lever, Fabiano and Mayer, Dennis and Metje, Jan and Alisauskas, Skirmantas and Calegari, Francesca and D{\"u}sterer, Stefan and Feifel, Raimund and Niebuhr, Mario and Manschwetus, Bastian and Kuhlmann, Marion and Mazza, Tommaso and Robinson, Matthew Scott and Squibb, Richard J. and Trabattoni, Andrea and Wallner, M{\aa}ns and Wolf, Thomas J. A. and G{\"u}hr, Markus}, title = {Core-level spectroscopy of 2-thiouracil at the sulfur L1 and L2,3 edges utilizing a SASE free-electron-laser}, series = {Molecules}, volume = {26}, journal = {Molecules}, number = {21}, publisher = {MDPI}, address = {Basel}, issn = {1420-3049}, pages = {11}, year = {2021}, 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.}, language = {en} } @article{MayerLeverGuehr2022, author = {Mayer, Dennis and Lever, Fabiano and G{\"u}hr, Markus}, title = {Data analysis procedures for time-resolved x-ray photoelectron spectroscopy at a SASE free-electron-laser}, series = {Journal of physics : B, Atomic, molecular and optical physics}, volume = {55}, journal = {Journal of physics : B, Atomic, molecular and optical physics}, number = {5}, publisher = {IOP Publ.}, address = {Bristol}, issn = {0953-4075}, doi = {10.1088/1361-6455/ac3c91}, pages = {9}, year = {2022}, abstract = {The random nature of self-amplified spontaneous emission (SASE) is a well-known challenge for x-ray core level spectroscopy at SASE free-electron lasers (FELs). Especially in time-resolved experiments that require a combination of good temporal and spectral resolution the jitter and drifts in the spectral characteristics, relative arrival time as well as power fluctuations can smear out spectral-temporal features. We present a combination of methods for the analysis of time-resolved photoelectron spectra based on power and time corrections as well as self-referencing of a strong photoelectron line. Based on sulfur 2p photoelectron spectra of 2-thiouracil taken at the SASE FEL FLASH2, we show that it is possible to correct for some of the photon energy drift and jitter even when reliable shot-to-shot photon energy data is not available. The quality of pump-probe difference spectra improves as random jumps in energy between delay points reduce significantly. The data analysis allows to identify coherent oscillations of 1 eV shift on the mean photoelectron line of 4 eV width with an error of less than 0.1 eV.}, language = {en} } @article{MayerLeverPicconietal.2022, author = {Mayer, Dennis and Lever, Fabiano and Picconi, David and Metje, Jan and Ališauskas, Skirmantas and Calegari, Francesca and D{\"u}sterer, Stefan and Ehlert, Christopher and Feifel, Raimund and Niebuhr, Mario and Manschwetus, Bastian and Kuhlmann, Marion and Mazza, Tommaso and Robinson, Matthew Scott and Squibb, Richard James and Trabattoni, Andrea and Wallner, M{\aa}ns and Saalfrank, Peter and Wolf, Thomas J. A. and G{\"u}hr, Markus}, title = {Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy}, series = {Nature Communications}, volume = {13}, journal = {Nature Communications}, publisher = {Springer Nature}, address = {Berlin}, issn = {2041-1723}, doi = {10.1038/s41467-021-27908-y}, pages = {9}, year = {2022}, abstract = {The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220-250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.}, language = {en} } @article{MayerMatthaeiHeueretal.2019, author = {Mayer, Dennis and Matthaei, Christian T. and Heuer, Axel and G{\"u}hr, Markus}, title = {Kagome-fiber prism compressor combination for Yb}, series = {Journal of optics}, volume = {21}, journal = {Journal of optics}, number = {2}, publisher = {IOP Publ. Ltd.}, address = {Bristol}, issn = {2040-8978}, doi = {10.1088/2040-8986/aafdf6}, pages = {6}, year = {2019}, abstract = {Spectral broadening in hollow-core fibers is an important tool for pulse compression of low-peak power laser pulses, especially for Yb-based lasers. Here, we present a pulse compression scheme to reduce the pulse duration of a commercial Yb:KGW laser operating at 100 kHz repetition rate and 40 mu J pulse energy from 390 to 38 fs. The spectral broadening is accomplished using a krypton-filled Kagome-type fiber. We report broadened spectra for variable Kr-pressures and input powers. At optimal settings of 8 bar Kr-pressure and 3.3 W input power, the bandwidth of the pulse at the -10 dB level increased from 9.5 to 85 nm corresponding to a Fourier limit of 26 fs. A simple SF10 prism compressor is used to reduce the accumulated chirp and shortens the fiber output from about 500 to 38 fs. In addition to the spectral broadening, a pressure dependent change of the polarization is observed.}, language = {en} } @article{MayerPicconiRobinsonetal.2022, author = {Mayer, Dennis and Picconi, David and Robinson, Matthew S. and G{\"u}hr, Markus}, title = {Experimental and theoretical gas-phase absorption spectra of thionated uracils}, series = {Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature}, volume = {558}, journal = {Chemical physics : a journal devoted to experimental and theoretical research involving problems of both a chemical and physical nature}, publisher = {Elsevier}, address = {Amsterdam}, issn = {0301-0104}, doi = {10.1016/j.chemphys.2022.111500}, pages = {9}, year = {2022}, abstract = {We present a comparative study of the gas-phase UV spectra of uracil and its thionated counterparts (2-thiouracil, 4-thiouracil and 2,4-dithiouracil), closely supported by time-dependent density functional theory calculations to assign the transitions observed. We systematically discuss pure gas-phase spectra for the (thio)uracils in the range of 200-400 nm (similar to 3.2-6.4 eV), and examine the spectra of all four species with a single theoretical approach. We note that specific vibrational modelling is needed to accurately determine the spectra across the examined wavelength range, and systematically model the transitions that appear at wavelengths shorter than 250 nm. Additionally, we find in the cases of 2-thiouracil and 2,4-dithiouracil, that the gas-phase spectra deviate significantly from some previously published solution-phase spectra, especially those collected in basic environments.}, language = {en} } @article{MetjeLeverMayeretal.2020, author = {Metje, Jan and Lever, Fabiano and Mayer, Dennis and Squibb, Richard James and Robinson, Matthew Scott and Niebuhr, Mario and Feifel, Raimund and D{\"u}sterer, Stefan and G{\"u}hr, Markus}, title = {URSA-PQ}, series = {Applied Sciences}, volume = {10}, journal = {Applied Sciences}, number = {21}, publisher = {MDPI}, address = {Basel}, issn = {2076-3417}, doi = {10.3390/app10217882}, pages = {13}, year = {2020}, 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 R{\"o}ntgenspektroskopie 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.}, language = {en} } @article{RobinsonNiebuhrLeveretal.2021, author = {Robinson, Matthew Scott and Niebuhr, Mario and Lever, Fabiano and Mayer, Dennis and Metje, Jan and G{\"u}hr, Markus}, title = {Ultrafast photo-ion probing of the ring-opening process in trans-stilbene oxide}, series = {Chemistry - a European journal}, volume = {27}, journal = {Chemistry - a European journal}, number = {44}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1521-3765}, doi = {10.1002/chem.202101343}, pages = {11418 -- 11427}, year = {2021}, abstract = {The ultrafast photo-induced ring opening of the oxirane derivative trans-stilbene oxide has been studied through the use of ultrafast UV/UV pump-probe spectroscopy by using photo-ion detection. Single- and multiphoton probe paths and final states were identified through comparisons between UV power studies and synchrotron-based vacuum ultraviolet (VUV) single-photon ionization studies. Three major time-dependent features of the parent ion (sub-450 fs decay, (1.5 +/- 0.2) ps, and >100 ps) were observed. These decays are discussed in conjunction with the primary ring-opening mechanism of stilbene oxide, which occurs through C-C dissociation in the oxirane ring. The appearance of fragments relating to the masses of dehydrogenated diphenylmethane (167 amu) and dehydrogenated methylbenzene (90 amu) were also investigated. The appearance of the 167 amu fragment could suggest an alternative ultrafast ring-opening pathway via the dissociation of one of the C-O bonds within the oxirane ring.}, language = {en} }