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  • 1. Angelova, G.
    et al.
    Ziemann, V.
    Meseck, A.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    van der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Hamberg, Mathias
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Boedewadt, J.
    Khan, S.
    Winter, A.
    Schlarb, H.
    Loehl, F.
    Saldin, E.
    Schneidmiller, E.
    Yurkov, M.
    Observation of two-dimensional longitudinal-transverse correlations in an electron beam by laser-electron interactions2008In: Physical Review Special Topics - Accelerators and Beams, E-ISSN 1098-4402, Vol. 11, no 7, article id 70702Article in journal (Refereed)
    Abstract [en]

    During the preparatory work for the optical-replica synthesizer experiment in the free-electron laser FLASH at DESY, we were able to superimpose a short, approximately 200 fs long pulse from a frequencydoubled mode-locked erbium laser with titanium-sapphire amplifier and an approximately 20 ps long electron bunch in an undulator. This induces an energy modulation in a longitudinal slice of the electron bunch. A magnetic chicane downstream of the undulator converts the energy modulation into a density modulation within the slice that causes the emission of coherent optical transition radiation from a silver-coated silicon screen. Varying the relative timing between electron and laser, we use a camera to record two-dimensional images of the slices as a function of the longitudinal position within the electron bunch.

  • 2. Berrah, Nora
    et al.
    Fang, Li
    Murphy, Brendan
    Osipov, Timur
    Ueda, Kiyoshi
    Kukk, Edwin
    Feifel, Raimund
    van der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Richter, Robert
    Prince, Kevin C.
    Bozek, John D.
    Bostedt, Christoph
    Wada, Shin-ichi
    Piancastelli, Maria N.
    Tashiro, Motomichi
    Ehara, Masahiro
    Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser2011In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 108, no 41, p. 16912-16915Article in journal (Refereed)
    Abstract [en]

    Theory predicts that double-core-hole (DCH) spectroscopy can provide a new powerful means of differentiating between similar chemical systems with a sensitivity not hitherto possible. Although DCH ionization on a single site in molecules was recently measured with double-and single-photon absorption, double-core holes with single vacancies on two different sites, allowing unambiguous chemical analysis, have remained elusive. Here we report that direct observation of double-core holes with single vacancies on two different sites produced via sequential two-photon absorption, using short, intense X-ray pulses from the Linac Coherent Light Source free-electron laser and compare it with theoretical modeling. The observation of DCH states, which exhibit a unique signature, and agreement with theory proves the feasibility of the method. Our findings exploit the ultrashort pulse duration of the free-electron laser to eject two core electrons on a time scale comparable to that of Auger decay and demonstrate possible future X-ray control of physical inner-shell processes.

  • 3. Hansen, Klavs
    et al.
    Richter, Robert
    Alagia, Michele
    Stranges, Stefano
    Schio, Luca
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Yatsyna, Vasyl
    Feifel, Raimund
    Zhaunerchyk, Vitali
    Single Photon Thermal Ionization of C-602017In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 118, no 10, article id 103001Article in journal (Refereed)
    Abstract [en]

    We report on experiments which show that C-60 can ionize in an indirect, quasithermal boiloff process after absorption of a single photon. The process involves a large number of incoherently excited valence electrons and yields electron spectra with a Boltzmann distribution with temperatures exceeding 10(4) K. It is expected to be present for other molecules and clusters with a comparatively large number of valence electrons. The astrophysical consequences are briefly discussed.

  • 4.
    Larsson, Mats
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    van der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Schmidt, Henning T.
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Feifel, R.
    Piancastelli, M. N.
    Fang, L.
    Murphy, B. F.
    Osipov, T.
    Berrah, N.
    Kukk, E.
    Ueda, K.
    Bozek, J. D.
    Bostedt, C.
    Wada, S.
    Richter, R.
    Feyer, V.
    Prince, K. C.
    Double core-hole formation in small molecules at the LCLS free electron laser2013In: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 46, no 16, p. 164030-Article in journal (Refereed)
    Abstract [en]

    We have investigated nonlinear processes in small molecules by x-ray photoelectron spectroscopy using the Linac Coherent Light Source free electron laser, and by simulations. The main focus of the experiments was the formation of the two-site double core-hole (tsDCH) states in the molecules CO2, N2O and N-2. These experiments are described in detail and the results are compared with simulations of the photoelectron spectra. The double core-hole states, and in particular the tsDCH states, have been predicted to be highly sensitive to the chemical environment. The theory behind this chemical sensitivity is validated by the experiments. Furthermore, our simulations of the relative integrated intensities of the peaks associated with the nonlinear processes show that this type of simulation, in combination with experimental data, provides a useful tool for estimating the duration of ultra-short x-ray pulses.

  • 5. Li, Cui
    et al.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Yatsyna, Vasyl
    Schio, Luca
    Feifel, Raimund
    Squibb, Richard
    Kaminska, Magdalena
    Stockholm University, Faculty of Science, Department of Physics. Jan Kochanowski University, Poland.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Richter, Robert
    Alagia, Michele
    Stranges, Stefano
    Monti, Susanna
    Carravetta, Vincenzo
    Zhaunerchyk, Vitali
    Experimental and theoretical XPS and NEXAFS studies of N-methylacetamide and N-methyltrifluoroacetamide2016In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 3, p. 2210-2218Article in journal (Refereed)
    Abstract [en]

    Experimental Near-Edge X-ray Absorption Fine-Structure (NEXAFS) spectra of N-methyltrifluoroacetamide (FNMA), which is a peptide model system, measured at the C, N, O and F K-edges are reported. The features in the spectra have been assigned by Static-Exchange (STEX) calculations. Using the same method, we have also assigned previously measured NEXAFS spectra of another peptide model system, N-methylacetamide (NMA). To facilitate the NEXAFS feature assignments, X-ray Photoelectron Spectroscopy (XPS) measurements for NMA and FNMA have been carried out with the aim of obtaining the 1s electron ionization potentials, which are compared with the values predicted by our Hartree-Fock (Delta HF) and Multi Configuration Self Consistent Field (Delta MCSCF) calculations. We also demonstrate an approach to compensate for screening effects that are neglected in the STEX method. Ion yield measurements of FNMA associated with the excitation of several C, N, O, and F K-shell pre-edge resonances have revealed site-specific fragmentation in some cases which we interpret with the aid of our theoretical calculations.

  • 6. Mak, Alan
    et al.
    Shamuilov, Georgii
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics. Uppsala University, Sweden.
    Dunning, David
    Hebling, Janos
    Kida, Yuichiro
    Kinjo, Ryota
    McNeil, Brian W. J.
    Tanaka, Takashi
    Thompson, Neil
    Tibai, Zoltan
    Toth, Gyorgy
    Goryashko, Vitaliy
    Attosecond single-cycle undulator light: a review2019In: Reports on progress in physics (Print), ISSN 0034-4885, E-ISSN 1361-6633, Vol. 82, no 2, article id 025901Article, review/survey (Refereed)
    Abstract [en]

    Research at modern light sources continues to improve our knowledge of the natural world, from the subtle workings of life to matter under extreme conditions. Free-electron lasers, for instance, have enabled the characterization of biomolecular structures with sub-angstrom spatial resolution, and paved the way to controlling the molecular functions. On the other hand, attosecond temporal resolution is necessary to broaden our scope of the ultrafast world. Here we discuss attosecond pulse generation beyond present capabilities. Furthermore, we review three recently proposed methods of generating attosecond x-ray pulses. These novel methods exploit the coherent radiation of microbunched electrons in undulators and the tailoring of the emitted wavefronts. The computed pulse energy outperforms pre-existing technologies by three orders of magnitude. Specifically, our simulations of the proposed Soft X-ray Laser at MAX IV (Lund, Sweden) show that a pulse duration of 50-100 as and a pulse energy up to 5 mu J is feasible with the novel methods. In addition, the methods feature pulse shape control, enable the incorporation of orbital angular momentum, and can be used in combination with modern compact free-electron laser setups.

  • 7. Mucke, M.
    et al.
    Zhaunerchyk, Vitali
    Stockholm University, Faculty of Science, Department of Physics. Uppsala University, Sweden; University of Gothenburg, Sweden.
    Frasinski, L. J.
    Squibb, R. J.
    Siano, M.
    Eland, J. H. D.
    Linusson, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    vab der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Foucar, L.
    Ullrich, J.
    Motomura, K.
    Mondal, S.
    Ueda, K.
    Osipov, T.
    Fang, L.
    Murphy, B. F.
    Berrah, N.
    Bostedt, C.
    Bozek, J. D.
    Schorb, S.
    Messerschmidt, M.
    Glownia, J. M.
    Cryan, J. P.
    Coffee, R. N.
    Takahashi, O.
    Wada, S.
    Piancastelli, M. N.
    Richter, R.
    Prince, K. C.
    Feifel, R.
    Covariance mapping of two-photon double core hole states in C2H2 and C2H6 produced by an x-ray free electron laser2015In: New Journal of Physics, E-ISSN 1367-2630, Vol. 17, article id 073002Article in journal (Refereed)
    Abstract [en]

    Few-photon ionization and relaxation processes in acetylene (C2H2) and ethane (C2H6) were investigated at the linac coherent light source x-ray free electron laser (FEL) at SLAC, Stanford using a highly efficient multi-particle correlation spectroscopy technique based on a magnetic bottle. The analysis method of covariance mapping has been applied and enhanced, allowing us to identify electron pairs associated with double core hole (DCH) production and competing multiple ionization processes including Auger decay sequences. The experimental technique and the analysis procedure are discussed in the light of earlier investigations of DCH studies carried out at the same FEL and at third generation synchrotron radiation sources. In particular, we demonstrate the capability of the covariance mapping technique to disentangle the formation of molecular DCH states which is barely feasible with conventional electron spectroscopy methods.

  • 8.
    Salén, Peter
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Kaminska, Magdalena
    Stockholm University, Faculty of Science, Department of Physics. Uppsala University, Sweden; Jan Kochanowski University, Poland.
    Squibb, Richard J.
    Richter, Robert
    Alagia, Michele
    Stranges, Stefano
    van der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Eland, John H. D.
    Feifel, Raimund
    Zhaunerchyk, Vitali
    Selectivity in fragmentation of N-methylacetamide after resonant K-shell excitation2014In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 16, no 29, p. 15231-15240Article in journal (Refereed)
    Abstract [en]

    The fragmentation pattern of the peptide model system, N-methylacetamide, is investigated using ion time-of-flight (TOF) spectroscopy after resonant K-shell excitation. Corresponding near-edge X-ray absorption fine structure (NEXAFS) spectra recorded at high resolution at the C1s, N1s and O1s edges are presented. Analysis of the ion TOF data reveals a multitude of fragmentation channels and dissociation pathways. Comparison between the excitation of six different resonances in the vicinity of the C1s, N1s and O1s edges suggests evidence for site-selective bond breaking. In particular the breaking of the peptide bond and the N-C-alpha bond show a clear correlation with resonant excitation at the N1s edge. Also, stronger tendencies towards site-selective bond breaking are found for the generation of single ions compared with ion pairs. Analysis of angular distributions of ions from breakage of the peptide bond yields a fragmentation time of <400 fs.

  • 9.
    Salén, Peter
    et al.
    Stockholm University, Faculty of Science, Department of Physics. Uppsala University, Sweden.
    Schio, Luca
    Richter, Robert
    Alagia, Michele
    Stranges, Stefano
    Zhaunerchyk, Vitali
    Investigating core-excited states of nitrosyl chloride (ClNO) and their break-up dynamics following Auger decay2018In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 149, no 16, article id 164305Article in journal (Refereed)
    Abstract [en]

    The fragmentation of ClNO upon resonant core-electron excitation to the LUMO and LUMO+1 orbitals at the N and O K-edges is investigated. The produced fragment ions were detected in coincidence with a position sensitive ion time-of-flight detector which enables deduction of the angular distribution of the ions. This facilitates a comparison between the two resonances and the two Kedges with respect to fragmentation time, transition dipole moment orientation, fragment yield of single-ion and ion-pair channels, and fragmentation mechanisms. We observe significant correlations between the core-excited site and the location of the bonds that are broken, as well as the dissociation time. Moreover, we observe preferential cleavage of specific bonds upon excitation to the LUMO and LUMO+1 states which can be attributed to their orbital character.

  • 10.
    Salén, Peter
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Yatsyna, Vasyl
    Schio, Luca
    Feifel, Raimund
    af Ugglas, Magnus
    Stockholm University, Faculty of Science, Department of Physics.
    Richter, Robert
    Alagia, Michele
    Stranges, Stefano
    Zhaunerchyk, Vitali
    Complete dissociation branching fractions and Coulomb explosion dynamics of SO2 induced by excitation of O 1s pre-edge resonances2015In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 143, no 13, article id 134302Article in journal (Refereed)
    Abstract [en]

    Fragmentation processes of SO2 following excitation of the six main O 1s pre-edge resonances, as well as above the ionization threshold and below the resonances, are studied using a position-sensitive time-of-flight ion imaging detector, and the associated dissociation branching ratios and break-up dynamics are determined. In order to distinguish between the O+ and S2+ fragments of equal mass-to-charge ratio, the measurements have been performed with the isotopically enriched (SO2)-O-18 sample. By analysis of the complete set of the fragment momentum vectors, the beta values for the fragments originating from the SO+ + O+ break-up and the kinetic energy release for fragmentation channels of both SO22+ and SO23+ parent ions are determined. We also present results on the three-body break-up dynamics.

  • 11.
    Salén, Peter
    et al.
    Stockholm University, Faculty of Science, Department of Physics.
    Yatsyna, Vasyl
    Schio, Luca
    Feifel, Raimund
    Richter, Robert
    Alagia, Michele
    Stranges, Stefano
    Zhaunerchyk, Vitali
    NEXAFS spectroscopy and site-specific fragmentation of N-methylformamide, N,N-dimethylformamide, and N,N-dimethylacetamide2016In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 144, no 24, article id 244310Article in journal (Refereed)
    Abstract [en]

    Near-edge X-ray absorption fine-structure (NEXAFS) spectra measured at the C, N, and O K-edges for three molecules containing the amide moiety, N-methylformamide (HCONHCH3), N,N-dimethylformamide (HCON(CH3)(2)), and N,N-dimethylacetamide (CH3CON(CH3)(2)) are presented. These molecules have similar structures and differ by the number of methyl groups located at the molecular ends. The fragmentation of these molecules after resonant excitation at different K-edge resonances is also investigated, using a 3D-ion imaging time-of-flight spectrometer. A comparison between the molecules with respect to the relative contributions of the fragments created upon excitation at distinct resonances reveals site-specific fragmentation. Further information about the character of the core-excitation and dissociation process is obtained from the angular distributions of the ion fragments.

  • 12. Schio, Luca
    et al.
    Li, Cui
    Monti, Susanna
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Yatsyna, Vasyl
    Feifel, Raimund
    Alagia, Michele
    Richter, Robert
    Falcinelli, Stefano
    Stranges, Stefano
    Zhaunerchyk, Vitali
    Carravetta, Vincenzo
    NEXAFS and XPS studies of nitrosyl chloride2015In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 17, no 14, p. 9040-9048Article in journal (Refereed)
    Abstract [en]

    The electronic structure of nitrosyl chloride (ClNO) has been investigated in the gas phase by X-ray Photoelectron (XPS) and Near Edge X-ray Absorption Fine Structure (NEXAFS) spectroscopy at the Cl 2p, Cl 2s, N 1s and O 1s edges in a combined experimental and theoretical study. The theoretical calculations at different levels of approximation predict ionization potential values in good agreement with the experimental data and allow us to assign the main features of the absorption spectra. An unexpected failure of the density functional model is, however, observed in the calculation of the Cl 2s binding energy, which is related to a large self-interaction error. Largely different photoabsorption cross-section patterns are experimentally observed in core excitations from the investigated quantum shells (n = 1, 2). This finding is confirmed by the oscillator strength distributions calculated at different absorption edges; in the case of the n = 2 shell the bands below the threshold are extremely weak and most of the absorption intensity is due to excitations in the continuum.

  • 13. Yatsyna, Vasyl
    et al.
    Bakker, Daniel J.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Feifel, Raimund
    Rijs, Anouk M.
    Zhaunerchyk, Vitali
    Infrared Action Spectroscopy of Low-Temperature Neutral Gas-Phase Molecules of Arbitrary Structure2016In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 117, no 11, article id 118101Article in journal (Refereed)
    Abstract [en]

    We demonstrate a technique for IR action spectroscopy that enables measuring IR spectra in a background-free fashion for low-temperature neutral gas-phase molecules of arbitrary structure. The method is exemplified experimentally for N-methylacetamide molecules in the mid-IR spectral range of 1000-1800 cm(-1), utilizing the free electron laser FELIX. The technique involves the resonant absorption of multiple mid-IR photons, which induces molecular dissociation. The dissociation products are probed with 10.49 eV vacuum ultraviolet photons and analyzed with a mass spectrometer. We also demonstrate the capability of this method to record, with unprecedented ease, mid-IR spectra for the molecular associates, such as clusters and oligomers, present in a molecular beam. In this way the mass-selected spectra of low-temperature gas-phase dimers and trimers of N-methylacetamide are measured in the full amide I-III range.

  • 14. Zhaunerchyk, V.
    et al.
    Kamińska, Magdalena
    Stockholm University, Faculty of Science, Department of Physics. Uppsala University, Sweden; Jan Kochanowski University, Poland.
    Mucke, M.
    Squibb, R. J.
    Eland, J. H. D.
    Piancastelli, M. N.
    Frasinski, L. J.
    Grilj, J.
    Koch, M.
    McFarland, B. K.
    Sistrunk, E.
    Gühr, M.
    Coffee, R. N.
    Bostedt, C.
    Bozek, J. D.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Meulen, Peter v. d.
    Stockholm University, Faculty of Science, Department of Physics.
    Linusson, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Foucar, L.
    Ullrich, J.
    Motomura, K.
    Mondal, S.
    Ueda, K.
    Richter, R.
    Prince, K. C.
    Takahashi, O.
    Osipov, T.
    Fang, L.
    Murphy, B. F.
    Berrah, N.
    Feifel, R.
    Disentangling formation of multiple-core holes in aminophenol molecules exposed to bright X-FEL radiation2015In: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 48, no 24, article id 244003Article in journal (Refereed)
    Abstract [en]

    Competing multi-photon ionization processes, some leading to the formation of double core hole states, have been examined in 4-aminophenol. The experiments used the linac coherent light source (LCLS) x-ray free electron laser, in combination with a time-of-flight magnetic bottle electron spectrometer and the correlation analysis method of covariance mapping. The results imply that 4-aminophenol molecules exposed to the focused x-ray pulses of the LCLS sequentially absorb more than two x-ray photons, resulting in the formation of multiple core holes as well as in the sequential removal of photoelectrons and Auger electrons (so-called PAPA sequences).

  • 15. Zhaunerchyk, V.
    et al.
    Mucke, M.
    Salén, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    van der Meulen, Peter
    Stockholm University, Faculty of Science, Department of Physics.
    Kaminska, M.
    Squibb, R. J.
    Frasinski, L. J.
    Siano, M.
    Eland, J. H. D.
    Linusson, Per
    Stockholm University, Faculty of Science, Department of Physics.
    Thomas, Richard D.
    Stockholm University, Faculty of Science, Department of Physics.
    Larsson, Mats
    Stockholm University, Faculty of Science, Department of Physics.
    Foucar, L.
    Ullrich, J.
    Motomura, K.
    Mondal, S.
    Ueda, K.
    Osipov, T.
    Fang, L.
    Murphy, B. F.
    Berrah, N.
    Bostedt, C.
    Bozek, J. D.
    Schorb, S.
    Messerschmidt, M.
    Glownia, J. M.
    Cryan, J. P.
    Coffee, R. N.
    Takahashi, O.
    Wada, S.
    Piancastelli, M. N.
    Richter, R.
    Prince, K. C.
    Feifel, R.
    Using covariance mapping to investigate the dynamics of multi-photon ionization processes of Ne atoms exposed to X-FEL pulses2013In: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 46, no 16, p. 164034-Article in journal (Refereed)
    Abstract [en]

    We report on a detailed investigation into the electron emission processes of Ne atoms exposed to intense femtosecond x-ray pulses, provided by the Linac Coherent Light Source Free Electron Laser (FEL) at Stanford. The covariance mapping technique is applied to analyse the data, and the capability of this approach to disentangle both linear and nonlinear correlation features which may be hidden on coincidence maps of the same data set is demonstrated. Different correction techniques which enable improvements on the quality of the spectral features extracted from the covariance maps are explored. Finally, a method for deriving characteristics of the x-ray FEL pulses based on covariance mapping in combination with model simulations is presented.

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