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52 results on '"Tatiana Marchenko"'

1. Nonstatistical behavior of the photoionization of spin–orbit doublets

Author

Maria Luiza M. Rocco, Gildas Goldsztejn, Renaud Guillemin, Marc Simon, Maria Novella Piancastelli, Pranawa C. Deshmukh, Oksana Travnikova, C. Rasadi Munasinghe, David Keating, I. Ismail, Steven T. Manson, Tatiana Marchenko, Jessica B. Martins, Dimitris Koulentianos, Ralph Püttner, Loic Journel, Denis Céolin, Freie Universität Berlin, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Moléculaires d'Orsay (ISMO), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), University of Gothenburg (GU), Argonne National Laboratory [Lemont] (ANL), Universidade Federal do Rio de Janeiro (UFRJ), Uppsala University, Georgia State University, and University System of Georgia (USG)

Subjects
Physics, [PHYS]Physics [physics], Branching fraction, Atom and Molecular Physics and Optics, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, Photoionization, Photon energy, Condensed Matter Physics, 01 natural sciences, Atomic and Molecular Physics, and Optics, relativistic effects, 010305 fluids & plasmas, Teoretisk kemi, interchannel coupling, 0103 physical sciences, Orbit (dynamics), [CHIM]Chemical Sciences, Atom- och molekylfysik och optik, Atomic physics, Theoretical Chemistry, 010306 general physics, Relativistic quantum chemistry, photoionization, Spin-½
Abstract

The photoionization branching ratios of spin–orbit doublets are studied both experimentally and theoretically at energies several keV above threshold. The results show significant relativistic effects for Ar 2p in the autoionizing region below the 1s threshold, and large many-body effects for Xe 3d and 4d in the vicinity of the L-shell thresholds. The branching ratios in Xe are also found to vary significantly over very broad multi-keV energy regions both above and below the inner-shell thresholds. In addition, the Ar 2p study confirms experimentally the decades-old theoretical prediction that the nonresonant branching ratio does not approach the statistical (nonrelativistic) value, and, in fact, progressively diverges from statistical with increasing photon energy.

Published
2021

2. Multi-slit-type interference in carbon 2s photoionization of polyatomic molecules: from a fundamental effect to structural parameters

Author

Gildas Goldsztejn, Piero Decleva, Tatiana Marchenko, Maria Novella Piancastelli, Aurora Ponzi, Minna Patanen, Renaud Guillemin, Marc Simon, Oksana Travnikova, Loic Journel, R. K. Kushawaha, Saikat Nandi, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Oulu, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Dipartimento di Scienze Chimiche e Farmaceutiche, and Università degli studi di Trieste

Subjects
Diffraction, Physics, Polyatomic ion, General Physics and Astronomy, 02 engineering and technology, Photoionization, 010402 general chemistry, 021001 nanoscience & nanotechnology, Interference (wave propagation), 01 natural sciences, Molecular physics, 0104 chemical sciences, photoionization, Multi-slit-type interference, propane, n-butane, isobutane, Double-slit experiment, Molecule, Molecular orbital, Density functional theory, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Physics::Chemical Physics, Physical and Theoretical Chemistry, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS
Abstract

In molecular photoemission, the analogue of the celebrated Young's double slit experiment is coherent electron emission from two equivalent atomic centers, giving rise to an interference pattern. Here multi-slit interference is investigated in inner-valence photoionization of propane, n- butane, isobutane and methyl peroxide. A more complex pattern is observed due to molecular orbital delocalization in polyatomic molecules, blurring the distinction between interference and diffraction. The potential to extract geometrical information is emphasized, as a more powerful extension of the EXAFS technique. Accurate reproduction of experimental features is obtained by simulations at the static Density Functional Theory level.

Published
2019

3. A von Hamos spectrometer based on highly annealed pyrolytic graphite crystal in tender x-ray domain

Author

Renaud Guillemin, Ralph Püttner, Régis Vacheresse, Loic Journel, Tatiana Marchenko, Marc Simon, Jérôme Palaudoux, Francis Penent, Moustafa Zmerli, Denis Céolin, Oksana Travnikova, Dimitris Koulentianos, I. Ismail, T. Marin, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Photon, Materials science, Physics::Instrumentation and Detectors, Astrophysics::High Energy Astrophysical Phenomena, Hard X-rays, Analytical chemistry, X-ray fluorescence, Synchrotron radiation, Free electron lasers, 01 natural sciences, 010305 fluids & plasmas, Crystal, Condensed Matter::Materials Science, Carbon based materials, 0103 physical sciences, Spectral resolution, 010306 general physics, Microchannel plate detectors, Instrumentation, ComputingMilieux_MISCELLANEOUS, Spectroscopy, Spectrometer, 500 Naturwissenschaften und Mathematik::530 Physik::539 Moderne Physik, X-ray, Crystal optics, Beamline, Physics::Accelerator Physics, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Annealed pyrolytic graphite, Crystal orientation
Abstract

We have built an x-ray spectrometer in a von Hamos configuration based on a highly annealed pyrolytic graphite crystal. The spectrometer is designed to measure x-ray emission in the range of 2���5 keV. A spectral resolution E/��E of 4000 was achieved by recording the elastic peak of photons issued from the GALAXIES beamline at the SOLEIL synchrotron radiation facility.

Published
2021

4. The O K −2 V spectrum of CO: the influence of the second core-hole

Author

Ralph Püttner, Oksana Travnikova, Stéphane Carniato, J. Martins, Dimitris Koulentianos, I. Ismail, Tatiana Marchenko, Denis Céolin, L. Journel, Raimund Feifel, Maria Novella Piancastelli, Renaud Guillemin, Marc Simon, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), University of Gothenburg (GU), Freie Universität Berlin, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), and Uppsala University

Subjects
Photoemission spectroscopy, Double ionization, Atom and Molecular Physics and Optics, Electron shell, Ab initio, General Physics and Astronomy, 01 natural sciences, Resonance (particle physics), Molecular physics, Electron spectroscopy, Physical Chemistry, spectrum, 0103 physical sciences, Atom, Physical and Theoretical Chemistry, 010306 general physics, O atom, Physics, Fysikalisk kemi, [PHYS]Physics [physics], 010304 chemical physics, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, Potential energy, CO, Atom- och molekylfysik och optik
Abstract

International audience; Using synchrotron radiation in the tender X-ray regime, a photoelectron spectrum showing the formation of single site double-core-hole pre-edge states, involving the K shell of the O atom in CO, has been recorded by means of high-resolution electron spectroscopy. The experimentally observed structures have been simulated, interpreted and assigned, employing state-of-the-art ab initio quantum chemical calculations, on the basis of a theoretical model, accounting for their so-called direct or conjugate character. Features appearing above the double ionization threshold have been reproduced by taking into account the strong mixing between multi-excited and continuum states. The shift of the σ* resonance below the double ionization threshold, in combination with the non-negligible contributions of multi-excited configurations in the final states reached, gives rise to a series of avoided crossings between the different potential energy curves.

Published
2021

5. Argon KLL Auger spectrum: Initial states, core-hole lifetimes, shake, and knock-down processes

Author

Maria Novella Piancastelli, Satoshi Kosugi, Gildas Goldsztejn, Renaud Guillemin, Yoshiro Azuma, Ralph Püttner, Mateja Hrast, Marc Simon, Denis Céolin, Moustafa Zmerli, Tatiana Marchenko, Alexsandre F. Lago, Matjaz Žitnik, Loic Journel, Philippe Holzhey, Dimitris Koulentianos, Oksana Travnikova, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SOLEIL), Institut für Experimentalphysik, Freie Universität Berlin, Sorbonne Université (SU), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Physics, Auger electron spectroscopy, Angular momentum, Argon, [PHYS.PHYS.PHYS-ATOM-PH]Physics [physics]/Physics [physics]/Atomic Physics [physics.atom-ph], Photoemission spectroscopy, Astrophysics::High Energy Astrophysical Phenomena, chemistry.chemical_element, 01 natural sciences, Spectral line, 010305 fluids & plasmas, Auger, chemistry, Atomic electron transition, Excited state, 0103 physical sciences, [CHIM]Chemical Sciences, Atomic physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS
Abstract

State-of-the-art argon $KLL$ Auger spectra measured using photon energies of $h\ensuremath{\nu}=3216$ and 3400 eV are presented along with an Ar $[1s]$ photoelectron spectrum (square brackets indicate holes in the respective orbital). The two different photon energies used for measuring the Auger spectra allow distinguishing between the shake transitions during the Auger decay and the Auger transitions of the photoelectron satellites. A complete assignment of satellite transitions is provided, partially based on configuration-interaction calculations. In addition, Ar $[1s3(s,p)]{n}^{\ensuremath{'}}{l}^{\ensuremath{'}}\ensuremath{\rightarrow}[2{p}^{2}{(}^{1}{D}_{2})]$ transitions are observed, which can be explained by knock-down transitions leading to a direct exchange of angular momentum between the excited electron and the Auger electron. The lifetime broadenings of the Ar $[2s]$ single-core-hole state and the $[2{s}^{2}]$ and $[2s2p]$ double-core-hole states are also determined, confirming previously observed trends for double-core-hole states.

Published
2020

6. Single and multiple excitations in double-core-hole states of free water molecules

Author

Renaud Guillemin, Maria Novella Piancastelli, M. Simon, Stéphane Carniato, Denis Céolin, J. Martins, I. Ismail, Gildas Goldsztejn, Tatiana Marchenko, Dimitris Koulentianos, Oksana Travnikova, Ralph Püttner, L. Journel, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Instituto Português de Investigação do Mar e da Atmosfera (IPMA), and Sorbonne Université (SU)

Subjects
Binding energy, water, electron spectroscopy, 02 engineering and technology, 01 natural sciences, Electron spectroscopy, Molecular physics, double-corehole, 0103 physical sciences, Molecule, [CHIM]Chemical Sciences, HAXPES, 010306 general physics, Physics, [PHYS]Physics [physics], 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Atomic and Molecular Physics, and Optics, Core (optical fiber), hard x-rays, Excited state, Absorption (chemistry), Ionization energy, 0210 nano-technology, shake-up processes, Excitation, dissociation dynamics
Abstract

We present a combined experimental and theoretical study of the double-core-hole photoelectron spectrum obtained in isolated water molecules irradiated with hard x-rays above the oxygen K −2 threshold. States of the type O K −2 V and multiply excited states are created by single-photon absorption and subsequent one-electron emission. A detailed analysis enabled by high experimental resolution reveals dissociative nuclear dynamics in the K −2 V pre-edge states. At the binding energies above the K −2 double-ionization potential, a complex spectral pattern is observed and attributed to highly excited states involving multiple shake-up excitation processes with the aid of state-of-the-art theoretical calculations. A strong broadening due to the nuclear motion indicates a highly dissociative nature of these multiply excited states, in agreement with the theoretical analysis.

Published
2020

7. Conjugate photoelectron recapture peaks in the high resolution Auger electron spectra following near-threshold Ar 2p photoionization

Author

Satoshi Kosugi, F. Hosseini, Maria Novella Piancastelli, Kenji Ito, Fumihiro Koike, John D. Bozek, Tatiana Marchenko, M. Simon, Emma Sokell, Yoshiro Azuma, Oksana Travnikova, J. Martins, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, [PHYS]Physics [physics], Auger electron spectroscopy, 010304 chemical physics, Auger effect, Photoionization, Condensed Matter Physics, 01 natural sciences, Electron spectroscopy, Atomic and Molecular Physics, and Optics, Auger, Photoexcitation, symbols.namesake, Excited state, 0103 physical sciences, symbols, Rydberg formula, Atomic physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS
Abstract

We have observed formation of Rydberg series superimposed on the Ar (L3M2,3M2,3) Auger electron spectral profile with photoexcitation just above the 2p-13/2 photoionization threshold. This is due to the recapture of photoelectrons induced by post-collision interaction (PCI) between the Auger electron and photoelectron: Ar+ 2p-13/2+e- →Ar+ 3p-2ml+e- . The intensity distribution of the angular momentum state resolved Rydberg peaks revealed prominent conjugate peaks due to angular momentum exchange between photoelectrons and Auger electrons in the process. In addition, we measured the 2p-13/2nl→3p-2ml+e- resonant Auger spectra with high resolution below the 2p-13/2 threshold. Our results showed that conjugate shake-up/down 2p-13/2nd→3p-2mp+e- processes are stronger than the direct 2p-13/2nd→3p-2ms, (m-1)d+e- processes in the spectator Auger processes, implying a strong angular momentum exchange effect between photoelectron and Auger electron.

Published
2020

8. Strong configuration interaction in the 3 p photoelectron spectrum of Kr

Author

Tatiana Marchenko, Maria Novella Piancastelli, Yoshiro Azuma, T. Nagayasu, Masaki Oura, Marc Simon, J. Martins, Fumihiro Koike, Kenji Ito, Tatsuo Gejo, John D. Bozek, J. R. Harries, Emma Sokell, F. Hosseini, Stephan Fritzsche, Oksana Travnikova, Satoshi Kosugi, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), and Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, [PHYS]Physics [physics], Electronic correlation, Photoemission spectroscopy, State (functional analysis), Configuration interaction, 01 natural sciences, 010305 fluids & plasmas, Ionization, 0103 physical sciences, Atomic physics, 010306 general physics, Anisotropy, Intensity (heat transfer), ComputingMilieux_MISCELLANEOUS
Abstract

We measured the Kr photoelectron spectrum in the region close to the $3p$ ionization threshold. Our high-resolution measurements allowed a clear observation of spectral structures due to electron correlation effects. Analysis based on relativistic multiconfiguration calculations could explain these observed peaks as due to strong configuration interactions between the $3{p}^{\ensuremath{-}1}$ state and $3{d}^{\ensuremath{-}2}nl$ states. Calculated and experimental data for peak assignments and intensity distributions are in good agreement. In addition, we measured the anisotropy parameter $\ensuremath{\beta}$, which also agreed well with theory. These findings provide a detailed view of strong configuration interactions between the $3{p}^{\ensuremath{-}1}$ and $3{d}^{\ensuremath{-}2}nl$ inner-shell hole states.

Published
2020

9. Hard x-ray spectroscopy and dynamics of isolated atoms and molecules: a review

Author

Renaud Guillemin, M. Simon, I. Ismail, L. Journel, Oksana Travnikova, Tatiana Marchenko, Maria Novella Piancastelli, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire des collisions atomiques et moléculaires (LCAM), and Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, X-ray spectroscopy, Astrophysics::High Energy Astrophysical Phenomena, Attosecond, Atoms in molecules, General Physics and Astronomy, Electron, Photoionization, 01 natural sciences, 7. Clean energy, 3. Good health, Photoexcitation, X-ray photoelectron spectroscopy, Ionization, 0103 physical sciences, [CHIM]Chemical Sciences, Atomic physics, 010306 general physics
Abstract

We present here a review of the most significant recent achievements in the field of HAXPES (HArd X-ray PhotoElectron Spectroscopy) on isolated atoms and molecules, and related spectroscopies. The possibility of conducting hard x-ray photoexcitation and photoionization experiments under state-of-the art conditions in terms of photon and electron kinetic energy resolution has become available only in the last few years. HAXPES has then produced structural and dynamical information at the level of detail already reached in the VUV and soft-x-ray ranges. The much improved experimental conditions have allowed extending to the hard x-ray range some methods well established in soft x-ray spectroscopies. Investigations of electron and nuclear dynamics in the femtosecond (fs, 10-15 sec) and even attosecond (as, 10-18 sec) regime have become feasible. Complex relaxation phenomena following deep-core ionization can now be enlightened in great detail. Other phenomena like e.g. recoil-induced effects are much more important in fast photoelectron emission, which can be induced by hard x-rays. Furthermore, a new kind of ionic states with double core holes can be observed by x-ray single-photon absorption. Future perspectives are also discussed.

Published
2020

10. Electron spectroscopy and dynamics of HBr around the Br 1s-1 threshold

Author

Maria Novella Piancastelli, I. Ismail, Renaud Guillemin, Loic Journel, Minna Patanen, Kari Jänkälä, Marko Huttula, Denis Céolin, Tatiana Marchenko, Yoshiro Azuma, Oksana Travnikova, Dimitris Koulentianos, Nacer Boudjemia, Marc Simon, Ralph Püttner, Satoshi Kosugi, University of Oulu, Department of Physics, Institut für Experimentalphysik, Freie Universität Berlin, Sorbonne Université (SU), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC), Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Absorption spectroscopy, Photoemission spectroscopy, Atom and Molecular Physics and Optics, General Physics and Astronomy, Electron, 01 natural sciences, Electron spectroscopy, Spectral line, 010305 fluids & plasmas, Auger, Ionization, 0103 physical sciences, decay channels, Physics::Atomic and Molecular Clusters, ultra-fast dissociation, galaxies beamline, Physical and Theoretical Chemistry, auger-spectra, 010306 general physics, photoionization, ComputingMilieux_MISCELLANEOUS, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, energies, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Atom- och molekylfysik och optik, Ionization energy, Atomic physics, photoelectron-spectroscopy, k-edge
Abstract

A comprehensive electron spectroscopic study combined with partial electron yield measurements around the Br 1s ionization threshold of HBr at approximately equal to 13.482 keV is reported. In detail, the Br 1s(-1) X-ray absorption spectrum, the 1s(-1) photoelectron spectrum as well as the normal and resonant KLL Auger spectra are presented. Moreover, the L-shell Auger spectra measured with photon energies below and above the Br 1s(-1) ionization energy as well as on top of the Br 1s(-1)sigma* resonance are shown. The latter two Auger spectra represent the second step of the decay cascade subsequent to producing a Br 1s(-1) core hole. The measurements provide information on the electron and nuclear dynamics of deep core-excited states of HBr on the femtosecond timescale. From the different spectra the lifetime broadening of the Br 1s(-1) single core-hole state as well as of the Br(2s(-2),2s(-1)2p(-1),2p(-2)) double core-hole states are extracted and discussed. The slope of the strongly dissociative HBr 2p(-2)sigma* potential energy curve is found to be about -13.60 eV angstrom(-1). The interpretation of the experimental data, and in particular the assignment of the spectral features in the KLL and L-shell Auger spectra, is supported by relativistic calculations for HBr molecule and atomic Br.

Published
2020

11. Relativistic and resonant effects in the ionization of heavy atoms by ultra-intense hard X-rays

Author

Bertold Krässig, Sébastien Boutet, Sebastian Carron, Tais Gorkhover, Robin Santra, Kiyoshi Ueda, Benjamin Erk, Benedikt Rudek, Christoph Bostedt, J. Correa, Stephen H. Southworth, Lutz Foucar, Marc Simon, Maximilian Bucher, C. S. Lehmann, Roberto Alonso-Mori, Daniel Rolles, Sang-Kil Son, Tatiana Marchenko, Cédric Bomme, Rebecca Boll, Ken R. Ferguson, Zoltan Jurek, Garth J. Williams, Koudai Toyota, Jason E. Koglin, Linda Young, Artem Rudenko, Max Planck Institute for Medical Research [Heidelberg], Max-Planck-Gesellschaft, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), SLAC National Accelerator Laboratory (SLAC), Stanford University, Linac Coherent Light Source (LCLS), Stanford University-Stanford University, School of Science and Technology, University of Camerino, Argonne National Laboratory [Lemont] (ANL), Graduate school of science, Hiroshima International University, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Center for Free-Electron Laser Science (CFEL), and Kansas State University

Subjects
Photon, Science, Astrophysics::High Energy Astrophysical Phenomena, General Physics and Astronomy, chemistry.chemical_element, 02 engineering and technology, 01 natural sciences, Article, General Biochemistry, Genetics and Molecular Biology, Ion, Xenon, Ionization, 0103 physical sciences, 010306 general physics, lcsh:Science, ComputingMilieux_MISCELLANEOUS, Physics, Range (particle radiation), Multidisciplinary, [PHYS.PHYS]Physics [physics]/Physics [physics], General Chemistry, 021001 nanoscience & nanotechnology, 3. Good health, chemistry, Femtosecond, lcsh:Q, ddc:500, Electron configuration, Atomic physics, 0210 nano-technology, Relativistic quantum chemistry
Abstract

An accurate description of the interaction of intense hard X-ray pulses with heavy atoms, which is crucial for many applications of free-electron lasers, represents a hitherto unresolved challenge for theory because of the enormous number of electronic configurations and relativistic effects, which need to be taken into account. Here we report results on multiple ionization of xenon atoms by ultra-intense (about 1019 W/cm2) femtosecond X-ray pulses at photon energies from 5.5 to 8.3 keV and present a theoretical model capable of reproducing the experimental data in the entire energy range. Our analysis shows that the interplay of resonant and relativistic effects results in strongly structured charge state distributions, which reflect resonant positions of relativistically shifted electronic levels of highly charged ions created during the X-ray pulse. The theoretical approach described here provides a basis for accurate modeling of radiation damage in hard X-ray imaging experiments on targets with high-Z constituents., Availability of intense hard X-ray pulses allows exploration of multiple ionization effects in heavier elements. Here, the authors measure the complex charge state distributions of xenon and found a reasonable agreement by comparing with the model including the relativistic and resonance effects.

Published
2018

12. Time-resolved ion imaging at free-electron lasers using TimepixCam

Author

Farzaneh Ziaee, Benjamin Erk, Andrei Nomerotski, Tatiana Marchenko, Merlin Fisher-Levine, Cédric Bomme, Daniel Rolles, Rebecca Boll, Dimitrios Rompotis, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Free electron model, Physics, Nuclear and High Energy Physics, CMOS sensor, Radiation, Pixel, business.industry, Fragment (computer graphics), Detector, 02 engineering and technology, Photoionization, 021001 nanoscience & nanotechnology, Laser, 01 natural sciences, Ion, law.invention, Optics, law, 0103 physical sciences, 010306 general physics, 0210 nano-technology, business, Instrumentation, ComputingMilieux_MISCELLANEOUS
Abstract

The application of a novel fast optical-imaging camera, TimepixCam, to molecular photoionization experiments using the velocity-map imaging technique at a free-electron laser is described. TimepixCam is a 256 × 256 pixel CMOS camera that is able to detect and time-stamp ion hits with 20 ns timing resolution, thus making it possible to record ion momentum images for all fragment ions simultaneously and avoiding the need to gate the detector on a single fragment. This allows the recording of significantly more data within a given amount of beam time and is particularly useful for pump–probe experiments, where drifts, for example, in the timing and pulse energy of the free-electron laser, severely limit the comparability of pump–probe scans for different fragments taken consecutively. In principle, this also allows ion–ion covariance or coincidence techniques to be applied to determine angular correlations between fragments.

Published
2018

13. Photoelectron–Auger-electron angular-momentum transfer in core-ionized Ar: Beyond the standard post-collision-interaction model

Author

Maria Novella Piancastelli, Benedikt Lassalle-Kaiser, Oksana Travnikova, S. Sheinerman, Moustafa Zmerli, Marc Simon, Leonid G. Gerchikov, Renaud Guillemin, Tatiana Marchenko, Loic Journel, T. Marin, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Saint Petersburg State Technical University, Saint Petersburg State Polytechnical University (SPSPU), Synchrotron SOLEIL (SSOLEIL), and Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, Angular momentum, Auger electron spectroscopy, Argon, [PHYS.PHYS.PHYS-ATOM-PH]Physics [physics]/Physics [physics]/Atomic Physics [physics.atom-ph], Physics::Instrumentation and Detectors, chemistry.chemical_element, Photoionization, Photoelectric effect, 01 natural sciences, Coincidence, 010305 fluids & plasmas, Ion, chemistry, Physics::Plasma Physics, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, Atomic physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS
Abstract

Electron-ion coincidence experimental data obtained following argon 1s photoionization are reported. Slow photoelectrons were measured in coincidence with Ar+ and Ar2+ ions, and the beta angular di ...

Published
2019

14. Si 1s −1 , 2s −1 and 2p −1 lifetime broadening of SiX 4 (X = F, Cl, Br, CH 3 ) molecules: SiF 4 anomalous behaviour reassessed

Author

Kiyoshi Ueda, Tatiana Marchenko, Maria Novella Piancastelli, Osamu Takahashi, Loic Journel, Renaud Guillemin, Denis Céolin, Alexsandre F. Lago, Marc Simon, Ralph Püttner, Gildas Goldsztejn, Institut für Experimentalphysik, Freie Universität Berlin, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), IMRAM, and Tohoku University [Sendai]

Subjects
Materials science, intraatomic auger electron decay, photoelectron spectroscopy, General Physics and Astronomy, 02 engineering and technology, 01 natural sciences, Spectral line, Electron transfer, Laser linewidth, X-ray photoelectron spectroscopy, 0103 physical sciences, Coulomb, Molecule, Physical and Theoretical Chemistry, ComputingMilieux_MISCELLANEOUS, Line (formation), Auger electron spectroscopy, 010304 chemical physics, electron transfer mediated decay, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, 021001 nanoscience & nanotechnology, lifetime broadening, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, 0210 nano-technology
Abstract

The Si 1s−1, Si 2s−1, and Si 2p−1 photoelectron spectra of the SiX4 molecules with X = F, Cl, Br, CH3 were measured. From these spectra the Si 1s−1 and Si 2s−1 lifetime broadenings were determined, revealing a significantly larger value for the Si 2s−1 core hole of SiF4 than for the same core hole of the other molecules of the sequence. This finding is in line with the results of the Si 2p−1 core holes of a number of SiX4 molecules, with an exceptionally large broadening for SiF4. For the Si 2s−1 core hole of SiF4 the difference to the other SiX4 molecules can be explained in terms of Interatomic Coulomb Decay (ICD)-like processes. For the Si 2p−1 core hole of SiF4 the estimated values for the sum of the Intraatomic Auger Electron Decay (IAED) and ICD-like processes are too small to explain the observed linewidth. However, the results of the given discussion render for SiF4 significant contributions from Electron Transfer Mediated Decay (ETMD)-like processes at least plausible. On the grounds of our results, some more molecular systems in which similar processes can be observed are identified.

Published
2019

15. Energy-dependent relative cross sections in carbon 1s photoionization:separation of direct shake and inelastic scattering effects in single molecules

Author

Fernando D. Vila, Tatiana Marchenko, Minna Patanen, Johan Söderström, Marc Simon, Oksana Travnikova, Leif J. Sæthre, Loic Journel, John J. Rehr, Denis Céolin, Svante Svensson, Piero Decleva, T. X. Carroll, Renaud Guillemin, Joshua J. Kas, Gildas Goldsztejn, Andreas Lindblad, Knut J. Børve, Nils Mårtensson, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), University of Oulu, Uppsala Universitet [Uppsala], Biorobotics Lab (University of Washington), University of Washington [Seattle], Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Keuka college, University of Bergen (UiB), Dipartimento di Scienze Chimiche e Farmaceutiche, and Università degli studi di Trieste

Subjects
Range (particle radiation), 010304 chemical physics, Chemistry, Shake, Photoionization, Photon energy, Inelastic scattering, 010402 general chemistry, 01 natural sciences, Molecular physics, 0104 chemical sciences, Condensed Matter::Soft Condensed Matter, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Intramolecular force, 0103 physical sciences, Theoretical chemistry, Molecule, Physical and Theoretical Chemistry
Abstract

International audience; We demonstrate that the possibility of monitoring relative photoionization cross sections over a large photon energy range allows us to study and disentangle shake processes and intramolecular inelastic scattering effects. In this gas-phase study, relative intensities of the carbon 1s photoelectron lines from chemically inequivalent carbon atoms in the same molecule have been measured as a function of the incident photon energy in the range of 300–6000 eV. We present relative cross sections for the chemically shifted carbon 1s lines in the photoelectron spectra of ethyl trifluoroacetate (the “ESCA” molecule). The results are compared with those of methyl trifluoroacetate and S-ethyl trifluorothioacetate as well as a series of chloro-substituted ethanes and 2-butyne. In the soft X-ray energy range, the cross sections show an extended X-ray absorption fine structure type of wiggles, as was previously observed for a series of chloroethanes. The oscillations are damped in the hard X-ray energy range, but deviations of cross-section ratios from stoichiometry persist, even at high energies. The current findings are supported by theoretical calculations based on a multiple scattering model. The use of soft and tender X-rays provides a more complete picture of the dominant processes accompanying photoionization. Such processes reduce the main photoelectron line intensities by 20–60%. Using both energy ranges enabled us to discern the process of intramolecular inelastic scattering of the outgoing electron, whose significance is otherwise difficult to assess for isolated molecules. This effect relates to the notion of the inelastic mean free path commonly used in photoemission studies of clusters and condensed matter.

Published
2019

16. Ultrafast nuclear dynamics in the doubly-core-ionized water molecule observed via Auger spectroscopy

Author

Denis Céolin, Maria Novella Piancastelli, Oksana Travnikova, I. Ismail, Renaud Guillemin, L. Journel, Dimitris Koulentianos, Tatiana Marchenko, Gildas Goldsztejn, Marc Simon, Ludger Inhester, Ralph Püttner, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Freie Universität Berlin, and RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN)

Subjects
Astrophysics::High Energy Astrophysical Phenomena, 01 natural sciences, law.invention, Hard x-ray photoelectron spectroscopy, Nuclear dynamics, law, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Molecule, ddc:530, Physics::Atomic Physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS, Astrophysics::Galaxy Astrophysics, Physics, Auger electron spectroscopy, 010304 chemical physics, Molecules, Synchrotron, Core (optical fiber), 13. Climate action, Semiclassical methods, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, Ultrashort pulse, Autoionization & Auger processes, Excitation
Abstract

We present a combined experimental and theoretical study of the Auger-emission spectrum following double core ionization and excitation of gas-phase water molecules with hard-x-ray synchrotron radiation above the O $K^{−2}$ threshold. We observe an indication of ultrafast proton motion occurring within the 1.5 fs lifetime of the double-core-hole (DCH) states in water. Furthermore, we have identified symmetric and antisymmetric dissociation modes characteristic for particular DCH states. Our results serve as a fundamental reference for state-of-the-art studies of DCH dynamic processes in liquid water both at synchrotron and free-electron-laser facilities.

Published
2018

17. From synchrotrons for XFELs: the soft x-ray near-edge spectrum of the ESCA molecule

Author

Mario Simon, Lan Cheng, Minna Patanen, Linda Young, Xuechen Zheng, Bart Oostenrijk, S. L. Sorensen, Christoph Bostedt, Gilles Doumy, O. Travnikova, Esko Kokkonen, Tatiana Marchenko, Stephen H. Southworth, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
absorption spectroscopy, Absorption spectroscopy, Atom and Molecular Physics and Optics, coupled-cluster methods, water, probe, 02 engineering and technology, x-ray spectroscopy, 01 natural sciences, Electron spectroscopy, NEXAFS, symbols.namesake, 0103 physical sciences, [CHIM]Chemical Sciences, Molecule, xanes, ComputingMilieux_MISCELLANEOUS, Physics, X-ray spectroscopy, atoms, Valence (chemistry), 010304 chemical physics, nexafs, core, excitation, 021001 nanoscience & nanotechnology, Condensed Matter Physics, XANES, Atomic and Molecular Physics, and Optics, excited electronic states, photoabsorption, Absorption edge, shell, Rydberg formula, symbols, Atomic physics, 0210 nano-technology
Abstract

A predictive understanding of soft x-ray near-edge absorption spectra of small molecules is an enduring theoretical challenge and of current interest for x-ray probes of molecular dynamics. We report the experimental absorption spectrum for the electron spectroscopy for chemical analysis (ESCA) molecule (ethyl trifluoroacetate) near the carbon 1s absorption edge between 285–300 eV. The ESCA molecule with four chemically distinct carbon sites has previously served as a theoretical benchmark for photoelectron spectra and now for photoabsorption spectra. We report a simple edge-specific approach for systematically expanding standard basis sets to properly describe diffuse Rydberg orbitals and the importance of triple excitations in equation-of-motion coupled-cluster calculations of the energy interval between valence and Rydberg excitations.

Published
2020

18. Argon 1s −2 Auger hypersatellites

Author

Ralph Puettner, Jiaolong Zeng, Tatiana Marchenko, Maria Novella Piancastelli, Yongjun Li, Marc Simon, Yoshiro Azuma, Satoshi Kosugi, Denis Céolin, Oksana Travnikova, Moustafa Zmerli, Renaud Guillemin, Dimitris Koulentianos, Loic Journel, Freie Universität Berlin, Hebei University, Sorbonne Université (SU), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), and Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, Auger electron spectroscopy, Argon, [PHYS.PHYS.PHYS-ATOM-PH]Physics [physics]/Physics [physics]/Atomic Physics [physics.atom-ph], 010304 chemical physics, Atom and Molecular Physics and Optics, 500 Naturwissenschaften und Mathematik::530 Physik::530 Physik, chemistry.chemical_element, Condensed Matter Physics, 01 natural sciences, Auger spectroscopy, Atomic and Molecular Physics, and Optics, Auger, chemistry, TheoryofComputation_ANALYSISOFALGORITHMSANDPROBLEMCOMPLEXITY, 0103 physical sciences, Atom- och molekylfysik och optik, HAXPES, double core hole, Atomic physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS
Abstract

The 1s −2 Auger hypersatellite spectrum of argon is studied experimentally and theoretically. In total, three transitions to the final states 1s −12p −2(2 S e ,2 D e ) and 1s −12s −1(1 S)2p −1(2 P o ) are experimentally observed. The lifetime broadening of the 1s −2 → 1s −12p −2(2 S e ,2 D e ) states is determined to be 2.1(4) eV. For the used photon energy of hν = 7500 eV a KK/K ionisation ratio of 2.5(3) × 10−4 is derived. Generally, a good agreement between the experimental and present theoretical energy positions, linewidths, and intensities is obtained.

Published
2020

19. Energy Transfer into Molecular Vibrations and Rotations by Recoil in Inner-Shell Photoemission

Author

Ralph Püttner, Marta Berholts, Renaud Guillemin, Oksana Travnikova, Denis Céolin, L. Journel, Kiyoshi Ueda, Maria Novella Piancastelli, I. Ismail, T. D. Thomas, Edwin Kukk, S. Granroth, Marc Simon, Tatiana Marchenko, Department of Physics and Astronomy [Turku], University of Turku, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Freie Universität Berlin, Institute of Multidisciplinary Research for Advanced Materials, and Tohoku University [Sendai]

Subjects
Atomic & molecular processes in external fields, Photoemission spectroscopy, Physics::Instrumentation and Detectors, Energy transfer, General Physics and Astronomy, Atomic & molecular structure, 7. Clean energy, 01 natural sciences, Recoil, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Inner shell, Physics::Atomic Physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS, Envelope (waves), Physics, 010304 chemical physics, ta114, Molecular spectra, Molecular vibration, Potential energy surfaces, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, Photoemission, Excitation, Energy (signal processing)
Abstract

A mixture of ${\mathrm{CF}}_{4}$ and CO gases is used to study photoelectron recoil effects extending into the tender x-ray region. In ${\mathrm{CF}}_{4}$, the vibrational envelope of the C $1s$ photoelectron spectrum becomes fully dominated by the recoil-induced excitations, revealing vibrational modes hidden from Franck-Condon excitations. In CO, using ${\mathrm{CF}}_{4}$ as an accurate energy calibrant, we determine the partitioning of the recoil-induced internal excitation energy between rotational and vibrational excitation. The observed rotational recoil energy is 2.88(28) times larger than the observed vibrational recoil energy, well in excess of the ratio of 2 predicted by the basic recoil model. The experiment is, however, in good agreement with the value of 2.68 if energy transfer via Coriolis coupling is included.

Published
2018

20. Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

Author

Claire Vallance, Jérôme Palaudoux, Stefan Düsterer, Marc Simon, Evgeny Savelyev, Tatiana Marchenko, Hansjochen Köckert, Kasra Amini, Jongmin Lee, Benjamin Erk, R. Guillemin, Marie Géléoc, Cédric Bomme, Per Johnsson, Sebastian Trippel, Nora Schirmel, David M. P. Holland, Francis Penent, Barbara Cunha de Miranda, Jonathan G. Underwood, Rebecca Boll, Pavel K. Olshin, Sadia Bari, Thomas Kierspel, Maria Novella Piancastelli, Jochen Küpper, Jan Lahl, Michael Burt, I. Ismail, Simone Techert, Serguei Patchkovskii, Sylvain Maclot, Alexander S. Gentleman, Gildas Goldsztejn, Artem Rudenko, Felix Brauße, Terence Mullins, Daniel Rolles, Mark Brouard, Oksana Travnikova, Thierry Ruchon, Andrey S. Mereshchenko, Bastian Manschwetus, Dimitrios Rompotis, Joss Wiese, Arnaud Rouzée, Pascal Lablanquie, Romain Géneaux, Stuart R. Mackenzie, Loïc Journel, Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), University of Oxford, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Structures BioMoléculaires (SBM), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Lund University [Lund], Center for Free-Electron Laser Science (CFEL), Universität Hamburg (UHH), Saint Petersburg State Polytechnical University (SPSPU), Department of Physics and Astronomy [Uppsala], Uppsala University, Kansas State University, Max-Planck-Institut für Biophysikalische Chemie - Max Planck Institute for Biophysical Chemistry [Göttingen], Max-Planck-Gesellschaft, Department of Physics and Astronomy [UCL London], University College of London [London] (UCL), ANR-14-CE32-0010,Xstase,Étude du moment angulaire de faisceaux lumineux XUV: synthèse et transferts(2014), ANR-16-CE30-0001,ATTOMEMUCHO,Dynamique électronique attoseconde dans les molécules organiques isolées par la spectroscopie 'core-hole clock'(2016), European Project: 238671,EC:FP7:PEOPLE,FP7-PEOPLE-ITN-2008,ICONIC(2009), European Project: 641789,H2020,H2020-MSCA-ITN-2014,MEDEA(2015), University of Oxford [Oxford], Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Chemical Physics (physics.chem-ph), Physics, 010304 chemical physics, Atom and Molecular Physics and Optics, Chemical structure, Photodissociation, technology, industry, and agriculture, FOS: Physical sciences, Configuration interaction, 01 natural sciences, Molecular physics, Dissociation (chemistry), 3. Good health, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, X-ray photoelectron spectroscopy, Ionization, Physics - Chemical Physics, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Molecule, ddc:530, Atom- och molekylfysik och optik, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 010306 general physics, Spectroscopy
Abstract

International audience; Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

Published
2018

21. Chemical Understanding of the Limited Site-Specificity in Molecular Inner-Shell Photofragmentation

Author

Sang-Kil Son, Robin Santra, Stacey L. Sorensen, Minna Patanen, Christoph Bostedt, Esko Kokkonen, Oksana Travnikova, Bart Oostenrijk, Stephen H. Southworth, Marc Simon, Ludger Inhester, Linda Young, Tatiana Marchenko, Eindhoven University of Technology [Eindhoven] (TU/e), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Nano and Molecular Systems Research Unit (NMSRU), University of Oulu, Argonne National Laboratory [Lemont] (ANL), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Center for Free-Electron Laser Science (CFEL), and Deutsches Elektronen-Synchrotron [Hamburg] (DESY)

Subjects
Ab initio, 02 engineering and technology, Electronic structure, 01 natural sciences, Dissociation (chemistry), Fragmentation (mass spectrometry), Core electron, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Molecule, ddc:530, General Materials Science, Physics::Atomic Physics, Physics::Chemical Physics, Physical and Theoretical Chemistry, 010306 general physics, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], Internal energy, Chemistry, 021001 nanoscience & nanotechnology, 3. Good health, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Chemical physics, 0210 nano-technology
Abstract

The journal of physical chemistry letters 9(5), 1156 - 1163 (2018). doi:10.1021/acs.jpclett.7b03235, In many cases fragmentation of molecules upon inner-shell ionization is very unspecific with respect to the initially localized ionization site. Often this finding is interpreted in terms of an equilibration of internal energy into vibrational degrees of freedom after Auger decay. We investigate the X-ray photofragmentation of ethyl trifluoroacetate upon core electron ionization at environmentally distinct carbon sites using photoelectron–photoion–photoion coincidence measurements and ab initio electronic structure calculations. For all four carbon ionization sites, the Auger decay weakens the same bonds and transfers the two charges to opposite ends of the molecule, which leads to a rapid dissociation into three fragments, followed by further fragmentation steps. The lack of site specificity is attributed to the character of the dicationic electronic states after Auger decay instead of a fast equilibration of internal energy., Published by ACS, Washington, DC

Published
2018

22. Interplay of complex decay processes after argon 1 s ionization

Author

Tatiana Marchenko, Maria Novella Piancastelli, Benedikt Lassalle-Kaiser, T. Marin, Kari Jänkälä, B. Cunha de Miranda, Marc Simon, Denis Céolin, L. Journel, I. Ismail, Gildas Goldsztejn, Oksana Travnikova, Renaud Guillemin, Ralph Püttner, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), University of Oulu, RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Fachbereich Physik [Berlin], Freie Universität Berlin, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Moléculaire et des Matériaux d'Orsay (ICMMO), Université Paris-Sud - Paris 11 (UP11)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), and Fachbereich Physik [Freie Univeristät Berlin] | Department of Physics [Freie Univeristät Berlin]

Subjects
Physics, Argon, 010304 chemical physics, [PHYS.PHYS]Physics [physics]/Physics [physics], Physics::Instrumentation and Detectors, chemistry.chemical_element, Synchrotron radiation, 01 natural sciences, chemistry, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Radiative transfer, Relaxation (physics), Physics::Atomic Physics, Atomic physics, 010306 general physics, Autoionization & Auger processes, ComputingMilieux_MISCELLANEOUS
Abstract

Complex decay pathways involving radiative and nonradiative relaxation after deep core-level ionization in argon are disentangled by a unique combination of several synchrotron radiation-based spectroscopic techniques. In particular, by comparing the results obtained from electron-ion coincidence, photon-ion coincidence, and x-ray emission measurements, we are able to distinguish the final ionic states produced in the cascade decay involving Kα and Kβ radiative decay and final ionic states produced by nonradiative cascade decay. High-resolution Auger electron spectroscopy is then used as a complementary tool to identify the LMM transitions contributing to the cascade decay. Ab initio calculations are performed to identify the electronic states involved in the LMM decay.

Published
2018

23. KL double core hole pre-edge states of HCl

Author

Renaud Guillemin, Marc Simon, Maria Novella Piancastelli, Raimund Feifel, Oksana Travnikova, Gildas Goldsztejn, Loic Journel, Denis Céolin, Dimitris Koulentianos, Tatiana Marchenko, Ralph Püttner, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Fachbereich Physik [Berlin], Freie Universität Berlin, Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), University of Gothenburg (GU), and Fachbereich Physik [Freie Univeristät Berlin] | Department of Physics [Freie Univeristät Berlin]

Subjects
Physics, [PHYS]Physics [physics], chemical physics, Binding energy, Ab initio, General Physics and Astronomy, 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Potential energy, Electron spectroscopy, Molecular physics, Core (optical fiber), symbols.namesake, Ionization, 0103 physical sciences, Rydberg formula, symbols, Physical and Theoretical Chemistry, 010306 general physics, 0210 nano-technology, Quantum, ComputingMilieux_MISCELLANEOUS
Abstract

The formation of double core hole pre-edge states of the form 1s-12p-1(1,3P)σ*,nl for HCl, located on the binding energy scale as deep as 3 keV, has been investigated by means of a high resolution single channel electron spectroscopy technique recently developed for the hard X-ray region. A detailed spectroscopic assignment is performed based on ab initio quantum chemical calculations and by using a sophisticated fit model comprising regular Rydberg series. Quantum defects for the different Rydberg series are extracted and the energies for the associated double core hole ionization continua are extrapolated. Dynamical information such as the lifetime width of these double-core-hole pre-edge states and the slope of the related dissociative potential energy curves are also obtained. In addition, 1s-12p-1V-1nlλn'l'λ' double shake-up transitions and double core hole states of the form 1s-12s-1(1,3S)σ*,4s are observed.

Published
2018

24. Coulomb explosion imaging of CH3I and CH2CII photodissociation dynamics

Author

Barbara Cunha de Miranda, Per Johnsson, Romain Géneaux, Stuart R. Mackenzie, I. Ismail, Hansjochen Köckert, David M. P. Holland, Dimitrios Rompotis, Marie Géléoc, Jérôme Palaudoux, Loic Journel, Jonathan G. Underwood, Farzaneh Ziaee, Jan Lahl, Robert Mason, Kasra Amini, Mark Brouard, Gildas Goldsztejn, Artem Rudenko, Stefan Düsterer, Sylvain Maclot, Maria Novella Piancastelli, Arnaud Rouzée, Thierry Ruchon, Daniel Rolles, Michael Burt, Jongmin Lee, Rebecca Boll, Oksana Travnikova, Andrey S. Mereshchenko, Joss Wiese, Sebastian Trippel, Marc Simon, Francis Penent, Felix Allum, Felix Brauße, Bastian Manschwetus, Simone Techert, Evgeny Savelyev, Tatiana Marchenko, Henrik Stapelfeldt, Renaud Guillemin, Nora Schirmel, Cédric Bomme, Benjamin Erk, Alexander S. Gentleman, Claire Vallance, Pavel K. Olshin, Sadia Bari, Jochen Küpper, University of Oxford, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Saint Petersburg State Polytechnical University (SPSPU), KVI Atomic and Molecular Physics (KVI), University of Groningen [Groningen], Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Attophysique (ATTO), Institut Rayonnement Matière de Saclay (IRAMIS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Laboratoire Interactions, Dynamiques et Lasers (ex SPAM) (LIDyl), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Microbiology Laboratory, Middlemore Hospital, Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Department of Physics, Lund Institute of Technology, Lund University [Lund]-Lund University [Lund], Lund University [Lund], Centre de recherche sur les Ions, les MAtériaux et la Photonique (CIMAP - UMR 6252), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Physical and Theoretical Chemistry Laboratory, Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB), Université de Bourgogne (UB)-Centre National de la Recherche Scientifique (CNRS), Kansas State University, Georg-August-University = Georg-August-Universität Göttingen, Department of Physics and Astronomy [UCL London], University College of London [London] (UCL), Center for Free-Electron Laser Science (CFEL), ANR-16-CE30-0001,ATTOMEMUCHO,Dynamique électronique attoseconde dans les molécules organiques isolées par la spectroscopie 'core-hole clock'(2016), University of Oxford [Oxford], Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interdisciplinaire Carnot de Bourgogne (LICB), Georg-August-University [Göttingen], Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Caen Normandie (UNICAEN), and Normandie Université (NU)

Subjects
Atom and Molecular Physics and Optics, Imaging spectrometer, General Physics and Astronomy, 02 engineering and technology, Physical Chemistry, 01 natural sciences, Molecular physics, Mass spectrometry imaging, Ion, 0103 physical sciences, Molecule, ddc:530, Physical and Theoretical Chemistry, 010306 general physics, ComputingMilieux_MISCELLANEOUS, Fysikalisk kemi, Physics, Coupling, Range (particle radiation), Photodissociation, Coulomb explosion, 021001 nanoscience & nanotechnology, 3. Good health, Atom- och molekylfysik och optik, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], 0210 nano-technology
Abstract

The journal of chemical physics 149(20), 204313 (2018). doi:10.1063/1.5041381, The photodissociation dynamics of CH$_3$I and CH$_2$ClI at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815 nm probe pulse. Fragment ion momenta over a wide m/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH$_2$ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion., Published by American Institute of Physics, Melville, NY

Published
2018

25. Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Author

Renaud Guillemin, Maria Novella Piancastelli, Alexander S. Gentleman, Artem Rudenko, Jérôme Palaudoux, Thierry Ruchon, O. Travnikova, Rebecca Boll, Felix Brausse, Rolf Treusch, Marc Simon, Arnaud Rouzée, Mark Brouard, Stefan Düsterer, Joss Wiese, Stuart R. Mackenzie, Jochen Küpper, Sebastian Trippel, Loic Journel, Jonathan G. Underwood, Claire Vallance, Michael Burt, Nora Schirmel, Kasra Amini, David M. P. Holland, Farzaneh Ziaee, Francis Penent, Benjamin Erk, Jan Lahl, Per Johnsson, Romain Géneaux, Barbara Cunha de Miranda, Hansjochen Köckert, Andrey S. Mereshchenko, Jongmin Lee, Marie Géléoc, Gildas Goldsztejn, Bastian Manschwetus, Sylvain Maclot, Henrik Stapelfeldt, Daniel Rolles, Cédric Bomme, Iyas Ismail, Simone Techert, Evgeny Savelyev, Tatiana Marchenko, Erland Müller, Dimitrios Rompotis, Pavel K. Olshin, and Sadia Bari

Subjects
Physics, Photon, Photodissociation, Coulomb explosion, 010402 general chemistry, medicine.disease_cause, Laser, 01 natural sciences, 0104 chemical sciences, Chemical Dynamics, law.invention, law, Ionization, 0103 physical sciences, Femtosecond, medicine, Atomic physics, 010306 general physics, Ultraviolet
Abstract

The dynamics following laser-induced molecular photodissociation of gas-phase CH2BrI at 271.6 nm were investigated by time-resolved Coulomb-explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH2BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH2Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb-explosion imaging as a real-time probe of chemical dynamics.

Published
2017

26. Electronic-state–lifetime interference in the hard-x-ray regime: Argon as a showcase

Author

R. K. Kushawaha, Marc Simon, Tatiana Marchenko, R. Guillemin, Ralph Püttner, Denis Céolin, L. Journel, B. Cunha de Miranda, Gildas Goldsztejn, Maria Novella Piancastelli, Oksana Travnikova, I. Ismail, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Fachbereich Physik [Berlin], Freie Universität Berlin, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Department of Astronomy and Space Physics [Uppsala], Uppsala University, and Fachbereich Physik [Freie Univeristät Berlin] | Department of Physics [Freie Univeristät Berlin]

Subjects
Physics, Argon, [PHYS.PHYS.PHYS-ATOM-PH]Physics [physics]/Physics [physics]/Atomic Physics [physics.atom-ph], 010304 chemical physics, Atoms in molecules, Relaxation (NMR), chemistry.chemical_element, 01 natural sciences, 7. Clean energy, Auger, Dipole, chemistry, Excited state, Ionization, 0103 physical sciences, Atomic physics, 010306 general physics, Excitation
Abstract

International audience; Electronic-state–lifetime interference is a phenomenon specific for ionization of atoms and molecules in the hard-x-ray regime. Using resonant KL 2,3 L 2,3 Auger decay in argon as a showcase, we present a model that allows extracting the interference terms directly from the cross sections of the final electronic states. The analysis provides fundamental information on the excitation and decay processes such as probabilities of various decay paths and the values of the dipole matrix elements for transitions to the excited states. Our results shed light on the interplay between spectator, shake-down, and shake-up processes in the relaxation of deep core-hole states.

Published
2017

27. Detailed assignment of normal and resonant Auger spectra of Xe near the L edges

Author

Ralph Püttner, Marc Simon, Renaud Guillemin, Gildas Goldsztejn, Alexsandre F. Lago, L. Journel, Oksana Travnikova, Denis Céolin, I. Ismail, Kari Jänkälä, B. Cunha de Miranda, R. K. Kushawaha, Maria Novella Piancastelli, and Tatiana Marchenko

Subjects
Physics, Electronic structure of atoms & molecules, Atom and Molecular Physics and Optics, chemistry.chemical_element, 01 natural sciences, Atomic, Spectral line, 010305 fluids & plasmas, Auger, Xenon, chemistry, Molecular & Optical, Atomic electron transition, Electronic transitions, 0103 physical sciences, Atom- och molekylfysik och optik, Atomic physics, 010306 general physics, Autoionization & Auger processes
Abstract

We present a comprehensive experimental and theoretical investigation on the LMM, LMN, and LNN normal Auger spectra of xenon, which reveal excellent agreement with theory when core-hole lifetimes of the two-hole final states are taken into account. Generally, the spectra turned out to be highly complex due to a strong overlap of the Auger transitions subsequent to 2s(1/2)(-1), 2p(1/2)(-1), and 2p(3/2)(-1) ionization. This overlap is due to the splitting of the three initial L core holes and the different final M and N core holes being on the same order of magnitude of several hundred eV. The Auger transitions are assigned in detail based on the theoretical results. Most of the MM, MN, and NN final states are described well based on jj coupling. In addition, we present a detailed assignment of the resonant LM45M45 Auger transition subsequent to the 2s -> 6p, 7p and 2p -> 5d, 6d excitations.

Published
2017

28. Experimental and theoretical study of the double-core-hole hypersatellite Auger spectrum of Ne

Author

Alexsandre F. Lago, L. Journel, Maria Novella Piancastelli, P. Selles, Renaud Guillemin, Stéphane Carniato, B. Cunha de Miranda, I. Ismail, Francis Penent, Denis Céolin, Tatiana Marchenko, Raimund Feifel, Gildas Goldsztejn, Oksana Travnikova, Pascal Lablanquie, Marc Simon, Ralph Püttner, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Fachbereich Physik [Freie Univeristät Berlin] | Department of Physics [Freie Univeristät Berlin], Freie Universität Berlin, RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut Lavoisier de Versailles (ILV), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Department of Physics, Uppsala University, Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC), and Fachbereich Physik [Berlin]

Subjects
Physics, [PHYS]Physics [physics], 010304 chemical physics, Spectrum (functional analysis), chemistry.chemical_element, 01 natural sciences, 3. Good health, Auger, Core (optical fiber), Neon, chemistry, Ionization, 0103 physical sciences, [CHIM]Chemical Sciences, Atomic physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS
Abstract

We present the hypersatellite Auger spectrum of neon which contains the decay transitions of the ${K}^{\ensuremath{-}2}, {K}^{\ensuremath{-}2}V, {K}^{\ensuremath{-}2}{L}^{\ensuremath{-}1}, {K}^{\ensuremath{-}2}{L}^{\ensuremath{-}1}V$, and ${K}^{\ensuremath{-}1}{L}^{\ensuremath{-}1}V$ states. The Auger decays of these types of core-hole states show different line shapes and linewidths which can be distinguished due to the high experimental resolution available for the present experiments. The individual Auger transitions are assigned based on various approaches. Complementary calculations are performed to assign the ${K}^{\ensuremath{-}2}{L}^{\ensuremath{-}1}\ensuremath{\rightarrow}{K}^{\ensuremath{-}1}{L}^{\ensuremath{-}3}$ and the ${K}^{\ensuremath{-}2}{L}^{\ensuremath{-}1}V\ensuremath{\rightarrow}{K}^{\ensuremath{-}1}{L}^{\ensuremath{-}3}V$ Auger transitions. Based on the obtained results we were able to derive the ratio for the double to single ionization yield.

Published
2017

29. Potential Energy Surface Reconstruction and Lifetime Determination of Molecular Double-Core-Hole States in the Hard X-Ray Regime

Author

Alexsandre F. Lago, B. Cunha de Miranda, Matjaž Žitnik, Ralph Püttner, Marc Simon, Nicolas Sisourat, Klemen Bučar, A. Mihelič, Kari Jänkälä, Renaud Guillemin, L. Journel, Faris Gel'mukhanov, Tatiana Marchenko, Denis Céolin, Matjaž Kavčič, Gildas Goldsztejn, Oksana Travnikova, Maria Novella Piancastelli, I. Ismail, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), University of Oulu, Jozef Stefan Institute [Ljubljana] (IJS), Universidade Federal do ABC (UFABC), Royal Institute of Technology [Stockholm] (KTH ), Freie Universität Berlin, Universidade Federal do ABC = Federal University of ABC = Université Fédérale de l'ABC [Brazil] (UFABC), and ANR-16-CE30-0001,ATTOMEMUCHO,Dynamique électronique attoseconde dans les molécules organiques isolées par la spectroscopie 'core-hole clock'(2016)

Subjects
Auger electron spectroscopy, Materials science, 010304 chemical physics, Scattering, Astrophysics::High Energy Astrophysical Phenomena, X-ray, General Physics and Astronomy, 01 natural sciences, Core (optical fiber), Excited state, 0103 physical sciences, Potential energy surface, Molecule, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, 010306 general physics
Abstract

International audience; A combination of resonant inelastic x-ray scattering and resonant Auger spectroscopy provides complementary information on the dynamic response of resonantly excited molecules. This is exemplified for CH3I, for which we reconstruct the potential energy surface of the dissociative I 3d−2 double-core-hole state and determine its lifetime. The proposed method holds a strong potential for monitoring the hard x-ray induced electron and nuclear dynamic response of core-excited molecules containing heavy elements, where ab initio calculations of potential energy surfaces and lifetimes remain challenging.

Published
2017

30. Subfemtosecond Control of Molecular Fragmentation by Hard X-Ray Photons

Author

Tatiana Marchenko, L. Journel, Renaud Guillemin, Ralph Püttner, Gildas Goldsztejn, Maria Novella Piancastelli, Marc Simon, I. Ismail, Alexsandre F. Lago, Oksana Travnikova, Denis Céolin, Nicolas Sisourat, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Centro de Ciencias Naturais e Humanas, Universidade Federal do ABC Santo André, and Freie Universität Berlin

Subjects
Physics, Wave packet, General Physics and Astronomy, 02 engineering and technology, Photon energy, 021001 nanoscience & nanotechnology, 01 natural sciences, Potential energy, Dissociation (chemistry), Auger, Fragmentation (mass spectrometry), 0103 physical sciences, Hard X-Ray Photons, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Atomic physics, 010306 general physics, 0210 nano-technology, Ultrashort pulse, Excitation
Abstract

International audience; Tuning hard x-ray excitation energy along Cl 1s→σ∗ resonance in gaseous HCl allows manipulating molecular fragmentation in the course of the induced multistep ultrafast dissociation. The observations are supported by theoretical modeling, which shows a strong interplay between the topology of the potential energy curves, involved in the Auger cascades, and the so-called core-hole clock, which determines the time spent by the system in the very first step. The asymmetric profile of the fragmentation ratios reflects different dynamics of nuclear wave packets dependent on the photon energy.

Published
2017

31. Photoelectron recoil in CO in the x-ray region up to 7 keV

Author

Maria Novella Piancastelli, Marc Simon, David Ayuso, Kuno Kooser, D. Iablonsky, Kiyoshi Ueda, S. Granroth, H. Levola, Oksana Travnikova, T. D. Thomas, Edwin Kukk, Ralph Püttner, Pietro Decleva, Denis Céolin, Tatiana Marchenko, Gildas Goldsztejn, Kukk, E., Thomas, T. D., Ueda, K., Céolin, D., Granroth, S., Kooser, K., Travnikova, O., Iablonsky, D., Decleva, Pietro, Ayuso, D., Püttner, R., Levola, H., Goldsztejn, G., Marchenko, T., Piancastelli, M. N., and Simon, M.

Subjects
Photon, Photoemission spectroscopy, Physics::Instrumentation and Detectors, 01 natural sciences, Molecular physics, Spectral line, Recoil, Atomic and Molecular Physics, Optics, 0103 physical sciences, Franck-Condon factorsIntensity ratio Photoelectron spectrum Potential energy curves Recoil effect Vibrational intensities Vibrational progressions X-ray energies, Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, Physics::Chemical Physics, 010306 general physics, Morse potential, Physics, Range (particle radiation), 010304 chemical physics, ta114, Rotational–vibrational spectroscopy, Coupling (probability), Atomic and Molecular Physic, Atomic physics
Abstract

Carbon $1s$ photoelectron spectra of CO molecules in gas phase were recorded in the tender x-ray energy range, from 2.3 to 6.9 keV. The intensity ratios of individual peaks from $\ensuremath{\nu}=0$ to 3 within the vibrational progression of the C $1s$ photoelectron spectrum were determined at the various photon energies and are shown to be strongly affected by the photoelectron recoil effect. The experimental vibrational intensity ratios are compared with theoretical predictions at different levels of accuracy. Developments of the recoil model, using generalized Franck-Condon factors, rovibrational coupling, Morse potential energy curves, and accurate angular averaging are presented and applied to the analysis of the experimental results.

Published
2017

32. Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

Author

Garth J. Williams, Rebecca Boll, Jason E. Koglin, Sang-Kil Son, M. Bucher, C. S. Lehmann, Koudai Toyota, Sébastien Boutet, Cédric Bomme, Christoph Bostedt, Sebastian Carron, Robin Santra, B. Kraessig, Tais Gorkhover, Benjamin Erk, Evgeny Savelyev, Tatiana Marchenko, J. Correa, Stephen H. Southworth, Marc Simon, Ludger Inhester, Benedikt Rudek, Oriol Vendrell, Kiyoshi Ueda, Ken R. Ferguson, Daniel Rolles, Y. Hao, Linda Young, S. J. Robatjazi, Xiang Li, Artem Rudenko, Kota Hanasaki, Lutz Foucar, and Roberto Alonso-Mori

Subjects
Time Factors, Protein Conformation, Static Electricity, Electrons, 02 engineering and technology, Electron, 01 natural sciences, Degree of ionization, ATOMS, Ionization, 0103 physical sciences, Atom, Molecule, FREE-ELECTRON LASERS, 010306 general physics, Photons, Multidisciplinary, Crystallography, Chemistry, Lasers, X-Rays, Polyatomic ion, Proteins, 021001 nanoscience & nanotechnology, PULSES, Kinetics, Heteronuclear molecule, Femtosecond, IONIZATION, Atomic physics, 0210 nano-technology, CHARGE, Iodine
Abstract

Upon exposure to ultra-intense, hard X-ray pulses, polyatomic molecules containing one heavy atom reach a much higher degree of ionization than do individual heavy atoms, contrary to previous assumptions. X-ray free-electron lasers offer many new applications such as the ability to structurally probe fast biological processes. This requires the use of hard and intense X-ray pulses, but the behaviour of matter under such conditions has not been fully explored. Artem Rudenko et al. show that when exposing small polyatomic molecules that contain one heavy atom to hard X-ray pulses with ultra-high intensities, the response is qualitatively different from what is seen in experiments carried out under less extreme conditions. The observed ionization of the molecule is considerably enhanced compared to that of an individual heavy atom under the same conditions, owing to ultrafast charge transfer within the molecule that replenishes the electrons removed from the heavy atom, enabling further ionization. Being able to account for this effect will aid further use of X-ray free-electron lasers for studying biological systems. X-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions1,2,3,4,5,6,7. Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 1020 watts per square centimetre)3,5. However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities8,9,10,11,12,13,14,15,16,17. Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption8,12,13,18, which in a heteronuclear molecular system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge14,15,16,17,19,20. In serial femtosecond crystallography of biological objects—an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure2,3—the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects21,22 and has been suggested as a way of phasing the diffraction data23,24. On the basis of experiments using either soft or less-intense hard X-rays14,15,16,17,18,19,25, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions. Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 1020 watts per square centimetre), hard (with photon energies of 8.3 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section. This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse. Our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible.

Published
2016

33. Double-Core-Hole States in Neon: Lifetime, Post-Collision Interaction, and Spectral Assignment

Author

Gildas Goldsztejn, Stéphane Carniato, P. Selles, Maria Novella Piancastelli, Francis Penent, Ralph Püttner, Raimund Feifel, Pascal Lablanquie, Alexsandre F. Lago, M. Simon, Renaud Guillemin, Denis Céolin, Loic Journel, Tatiana Marchenko, Oksana Travnikova, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Fachbereich Physik [Freie Univeristät Berlin] | Department of Physics [Freie Univeristät Berlin], Freie Universität Berlin, RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Department of Physics, Uppsala University, Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), and Fachbereich Physik [Berlin]

Subjects
Physics, [PHYS]Physics [physics], 010304 chemical physics, General Physics and Astronomy, chemistry.chemical_element, Synchrotron radiation, Electron, Photoelectric effect, 01 natural sciences, Electron spectroscopy, Auger, Neon, chemistry, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, [CHIM]Chemical Sciences, Physics::Atomic Physics, Atomic physics, 010306 general physics, Excitation, ComputingMilieux_MISCELLANEOUS
Abstract

Using synchrotron radiation and high-resolution electron spectroscopy, we have directly observed and identified specific photoelectrons from K^{-2}V states in neon corresponding to simultaneous 1s ionization and 1s→valence excitation. The natural lifetime broadening of the K^{-2}V states and the relative intensities of different types of shakeup channels have been determined experimentally and compared to ab initio calculations. Moreover, the high-energy Auger spectrum resulting from the decay of Ne^{2+}K^{-2} and Ne^{+}K^{-2}V states as well as from participator Auger decay from Ne^{+}K^{-1}L^{-1}V states, has been measured and assigned in detail utilizing the characteristic differences in lifetime broadenings of these core hole states. Furthermore, post collision interaction broadening of Auger peaks is clearly observed only in the hypersatellite spectrum from K^{-2} states, due to the energy sharing between the two 1s photoelectrons which favors the emission of one slow and one fast electron.

Published
2016

34. Photon-energy dependence of single-photon simultaneous core ionization and core excitation in CO 2

Author

Maria Novella Piancastelli, Denis Céolin, Gildas Goldsztejn, Stéphane Carniato, P. Selles, Francis Penent, Renaud Guillemin, Lidija Andric, Marc Simon, Jérôme Palaudoux, Kenji Ito, Yasumasa Hikosaka, Tatiana Marchenko, Pascal Lablanquie, Oksana Travnikova, L. Journel, M. Nakano, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Théorique (LCT), Université Paris-Est Marne-la-Vallée (UPEM), University of Toyama, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS)

Subjects
Physics, [PHYS]Physics [physics], 010304 chemical physics, Photon energy, 01 natural sciences, XANES, Spectral line, Vibronic coupling, Excited state, Ionization, 0103 physical sciences, [CHIM]Chemical Sciences, Absorption (logic), Atomic physics, 010306 general physics, Spectroscopy, ComputingMilieux_MISCELLANEOUS
Abstract

We have studied the ${K}^{\ensuremath{-}2}V$ process corresponding to simultaneous $K$-shell ionization and $K$-shell excitation in the $\mathrm{C}{\mathrm{O}}_{2}$ molecule. We define these ${K}^{\ensuremath{-}2}V$ states as super shake-up, at variance with the ``conventional'' ${K}^{\ensuremath{-}1}{v}^{\ensuremath{-}1}V$ shake-up states. While the nature and evolution with photon energy of the conventional shake-up satellites has been the object of many studies, no such data on a large photon-energy range were previously reported on super shake-up. The $\mathrm{C}{\mathrm{O}}_{2}$ molecule is a textbook example because it exhibits two well-isolated ${K}^{\ensuremath{-}2}V$ resonances (with V being $2{\ensuremath{\pi}}_{u}^{*}$ and $5{\ensuremath{\sigma}}_{g}^{*}$) with different symmetries resulting from shake-up processes of different origin populated in comparable proportions. The variation of the excitation cross section of these two resonances with photon energy is reported, using two different experimental approaches, which sheds light on the excitation mechanisms. Furthermore, double-core-hole spectroscopy is shown to be able to integrate and even expand information provided by conventional single-core-hole X-ray Photoelectron Spectroscopy (XPS) and Near-Edge X-ray Absorption Fine Structure (NEXAFS) techniques, revealing, for instance, $g\ensuremath{-}g$ dipole forbidden transitions which are only excited in NEXAFS spectra through vibronic coupling.

Published
2016

35. Hard-X-Ray-Induced Multistep Ultrafast Dissociation

Author

Eiji Shigemasa, Stéphane Carniato, Tatiana Marchenko, Kari Jänkälä, Denis Céolin, Renaud Guillemin, Hiroshi Iwayama, Maria Novella Piancastelli, Ralph Püttner, Gildas Goldsztejn, Oksana Travnikova, M. Simon, Nicolas Sisourat, Loic Journel, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Department of Physics, University of Oulu, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut für Experimentalphysik, Freie Universität Berlin, Ultraviolet Synchrotron Orbital Radiation Facility (UVSOR), Institute for Molecular Science, and Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC)

Subjects
[PHYS]Physics [physics], Materials science, Photon, 010304 chemical physics, X-ray, General Physics and Astronomy, 01 natural sciences, Potential energy, Molecular physics, Dissociation (chemistry), Fragmentation (mass spectrometry), Core electron, 0103 physical sciences, Physics::Atomic and Molecular Clusters, [CHIM]Chemical Sciences, 010306 general physics, Ultrashort pulse, ComputingMilieux_MISCELLANEOUS, Excitation
Abstract

Creation of deep core holes with very short (τ≤1 fs) lifetimes triggers a chain of relaxation events leading to extensive nuclear dynamics on a few-femtosecond time scale. Here we demonstrate a general multistep ultrafast dissociation on an example of HCl following Cl 1s→σ^{*} excitation. Intermediate states with one or multiple holes in the shallower core electron shells are generated in the course of the decay cascades. The repulsive character and large gradients of the potential energy surfaces of these intermediates enable ultrafast fragmentation after the absorption of a hard x-ray photon.

Published
2016

36. Electronic state-lifetime interference in resonant Auger spectra: a tool to disentangle overlapping core-excited states

Author

Renaud Guillemin, Maria Novella Piancastelli, Denis Céolin, M. Simon, Tatiana Marchenko, Loic Journel, Jean-Pascal Rueff, R. K. Kushawaha, Gildas Goldsztejn, and Ralph Püttner

Subjects
010304 chemical physics, Chemistry, General Physics and Astronomy, Shake, Interference (wave propagation), 01 natural sciences, Spectral line, Auger, Core (optical fiber), Excited state, 0103 physical sciences, Molecule, Physical and Theoretical Chemistry, Atomic physics, 010306 general physics, Ultrashort pulse
Abstract

We have measured resonant-Auger decay following Cl 1s(-1) excitations in HCl and CH3Cl molecules, and extracted the pseudo-cross sections of different Cl 2p(-2) final states. These cross sections show clear evidence of shake processes as well as contributions of electronic state-lifetime interference (ELI). To describe the spectra we developed a fit approach that takes into account ELI contributions and ultrafast nuclear dynamics in dissociative core-excited states. Using this approach we utilized the ELI contributions to obtain the intensity ratios of the overlapping states Cl 1s(-1)4pπ/1s(-1)4pσ in HCl and Cl 1s(-1)4pe/1s(-1)4pa1 in CH3Cl. The experimental value for HCl is compared with theoretical results showing satisfactory agreement.

Published
2016

37. Structural and dynamical properties of chlorinated hydrocarbons studied with resonant inelastic x-ray scattering

Author

M. Kavčič, M. Simon, Stéphane Carniato, Matjaž Žitnik, L. Journel, Renaud Guillemin, Wei Cao, Tatiana Marchenko, Klemen Bučar, E. Kawerk, R. Bohinc, Jozef Stefan Institute [Ljubljana] (IJS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), Department of Physics [Hong Kong University of Science and Technology], and Hong Kong University of Science and Technology (HKUST)

Subjects
[PHYS]Physics [physics], 010304 chemical physics, Scattering, Chemistry, General Physics and Astronomy, 01 natural sciences, Fluorescence, Spectral line, Resonant inelastic X-ray scattering, Distribution (mathematics), Position (vector), Yield (chemistry), 0103 physical sciences, Molecule, [CHIM]Chemical Sciences, Physics::Chemical Physics, Physical and Theoretical Chemistry, Atomic physics, 010306 general physics, ComputingMilieux_MISCELLANEOUS
Abstract

We present a theoretical and experimental study of resonant inelastic x-ray scattering on a large group of chlorinated hydrocarbons: CH3Cl, CH2Cl2, CHCl3, CCl4, CH3CH2Cl, ClCH2CH2Cl, CH3CHCl2, CH3CCl3, C2H2Cl2-iso, C2H2Cl2-cis, C2H2Cl2-trans, and C6H5Cl. Differences in structural and dynamical properties of the molecules generated by diverse chemical environments are observed in the measured Cl(K(α)) spectral maps as well as in the Cl(K) total fluorescence yield spectra. The energy position, relative intensity, and the width of the Franck-Condon distribution of low-lying σ* and π* resonances are extracted by a fitting procedure taking into account the experimental broadening. The theoretical values obtained with the transition potential and Δ Kohn-Sham methods are in good agreement with the experimental parameters indicating subtle differences due to variations in the molecular structure.

Published
2016

38. Detailed analysis of shake structures in theKLLAuger spectrum ofH2S

Author

Tatiana Marchenko, Maria Novella Piancastelli, R. K. Kushawaha, L. Journel, Denis Céolin, Renaud Guillemin, M. Simon, and Ralph Püttner

Subjects
Physics, 010304 chemical physics, Photoemission spectroscopy, 0103 physical sciences, Spectrum (functional analysis), Molecular orbital, Atomic physics, 010306 general physics, Lambda, Valence electron, 01 natural sciences, Spectral line, Auger
Abstract

Shake processes of different origin are identified in the $\mathit{KLL}$ Auger spectrum of ${\mathrm{H}}_{2}\mathrm{S}$ with unprecedented detail. The $\mathit{KLL}$ Auger spectrum is presented together with the S $1{s}^{\ensuremath{-}1}$ photoelectron spectrum including the S $1{s}^{\ensuremath{-}1}{V}^{\ensuremath{-}1}n\ensuremath{\lambda}$ and S $1{s}^{\ensuremath{-}1}2{p}^{\ensuremath{-}1}n\ensuremath{\lambda}$ shake-up satellites with ${V}^{\ensuremath{-}1}$ and $n\ensuremath{\lambda}$ indicating a hole in the valence shell and an unoccupied molecular orbital, respectively. By using different photon energies between 2476 and 4150 eV to record the $\mathit{KLL}$ Auger spectra two different shake-up processes responsible for the satellite lines are identified. The first process is a shake-up during the Auger decay of the S $1{s}^{\ensuremath{-}1}$ core hole and can be described by S $1{s}^{\ensuremath{-}1}\ensuremath{\rightarrow}2{p}^{\ensuremath{-}2}{V}^{\ensuremath{-}1}n\ensuremath{\lambda}$. The second process is the Auger decay of the shake-up satellite in the ionization process leading to S $1{s}^{\ensuremath{-}1}{V}^{\ensuremath{-}1}n\ensuremath{\lambda}\ensuremath{\rightarrow}2{p}^{\ensuremath{-}2}{V}^{\ensuremath{-}1}n\ensuremath{\lambda}$ transitions. By combining the results of photoelectron and Auger spectra the involved ${V}^{\ensuremath{-}1}n\ensuremath{\lambda}$ levels are assigned.

Published
2016

39. Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses

Author

Ken R. Ferguson, Ryan Coffee, John D. Bozek, Catalin Miron, M. Simon, Tatiana Marchenko, Timur Osipov, Cédric Bomme, Sebastian Schorb, Rebecca Boll, Thomas Kierspel, Sebastian Trippel, Lutz Foucar, Minna Patanen, M. Swiggers, Mitchell Burkett, Simone Techert, Daniel Rolles, Christoph Bostedt, Benjamin Erk, Jochen Küpper, Sebastian Carron, Artem Rudenko, Kiyoshi Ueda, Deutsches Elektronen-Synchrotron [Hamburg] (DESY), Max Planck Institute for Nuclear Physics (MPIK), Max-Planck-Gesellschaft, SLAC National Accelerator Laboratory (SLAC), Stanford University, Universität Hamburg (UHH), Kansas State University, Max Planck Institute for Medical Research [Heidelberg], Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Horia Hulubei National Institute of Physics and Nuclear Engineering (NIPNE), IFIN-HH, University of Oulu, Georg-August-University [Göttingen], Max Planck Institute for Biophysical Chemistry (MPI-BPC), IMRAM, Tohoku University [Sendai], Argonne National Laboratory [Lemont] (ANL), Northwestern University [Evanston], and Georg-August-University = Georg-August-Universität Göttingen

Subjects
Invited Articles, 02 engineering and technology, 01 natural sciences, Electron transfer, chemistry.chemical_compound, Ionization, 0103 physical sciences, lcsh:QD901-999, Fluoromethane, ddc:530, Physics::Chemical Physics, 010306 general physics, Instrumentation, Spectroscopy, [PHYS]Physics [physics], Radiation, Chemistry, Photodissociation, SPECIAL TOPIC: THE HAMBURG CONFERENCE ON FEMTOCHEMISTRY (FEMTO12), 021001 nanoscience & nanotechnology, Condensed Matter Physics, iodomethane, fluoromethane molecules, X-ray pulses, Photoexcitation, Intramolecular force, Femtosecond, lcsh:Crystallography, Atomic physics, 0210 nano-technology, Excitation
Abstract

International audience; Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse.

Published
2016

40. Two-to-one Auger decay of a double L vacancy in argon

Author

Maria Novella Piancastelli, Oksana Travnikova, M. Kavčič, M. Simon, Tatiana Marchenko, Ralph Püttner, L. Journel, Matjaž Žitnik, Renaud Guillemin, A. Mihelič, Gildas Goldsztejn, Denis Céolin, and Klemen Bučar

Subjects
Physics, Auger electron spectroscopy, Argon, 010304 chemical physics, Auger effect, Branching fraction, chemistry.chemical_element, 01 natural sciences, symbols.namesake, Internal conversion, chemistry, Atomic electron transition, Vacancy defect, 0103 physical sciences, symbols, Physics::Atomic and Molecular Clusters, High Energy Physics::Experiment, Atomic physics, 010306 general physics, Valence electron
Abstract

We have observed ${L}_{23}^{2}\ensuremath{-}{M}^{3}$ Auger decay in argon where a double vacancy is filled by two valence electrons and a single electron is ejected from the atom. A well-resolved spectrum of these two-to-one electron transitions is compared to the result of the second-order perturbation theory and its decay branching ratio is determined.

Published
2016

41. Double-core-hole states in CH3CN: Pre-edge structures and chemical-shift contributions

Author

Renaud Guillemin, Oksana Travnikova, Maria Luiza M. Rocco, Gildas Goldsztejn, Marc Simon, Dimitris Koulentianos, Denis Céolin, Stéphane Carniato, Ralph Püttner, Tatiana Marchenko, L. Journel, Raimund Feifel, Maria Novella Piancastelli, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Fachbereich Physik [Berlin], Freie Universität Berlin, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Department of Physics, and Uppsala University

Subjects
Materials science, Zero point energy, Hard X-rays, Ab initio, General Physics and Astronomy, chemistry.chemical_element, 01 natural sciences, Molecular physics, Spectral line, Photoelectron spectra, chemistry.chemical_compound, Correlation energy, X-ray photoelectron spectroscopy, 0103 physical sciences, [CHIM]Chemical Sciences, Quantum chemical calculations, Physical and Theoretical Chemistry, 010306 general physics, Acetonitrile, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], 010304 chemical physics, State (functional analysis), Core (optical fiber), Photoelectron spectroscopy, chemistry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Carbon, Excitation
Abstract

Spectra reflecting the formation of single-site double-core-hole pre-edge states involving the N 1s and C 1s core levels of acetonitrile have been recorded by means of high-resolution single-channel photoelectron spectroscopy using hard X-ray excitation. The data are interpreted with the aid of ab initio quantum chemical calculations, which take into account the direct or conjugate nature of this type of electronic states. Furthermore, the photoelectron spectra of N 1s and C 1s singly core-ionized states have been measured. From these spectra, the chemical shift between the two C 1s−1 states is estimated. Finally, by utilizing C 1s single and double core-ionization potentials, initial and final state effects for the two inequivalent carbon atoms have been investigated.

Published
2018

42. Experimental setup for the study of resonant inelastic X-ray scattering of organometallic complexes in gas phase

Author

I. Ismail, Marc Simon, Renaud Guillemin, Oksana Travnikova, Tatiana Marchenko, Maria Novella Piancastelli, Jean-Pascal Rueff, L. Journel, James M. Ablett, Laboratoire des collisions atomiques et moléculaires (LCAM), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Department of Physics, Uppsala University, Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS), and RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN)

Subjects
Materials science, [PHYS.PHYS]Physics [physics]/Physics [physics], Astrophysics::High Energy Astrophysical Phenomena, Synchrotron radiation, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Synchrotron, 0104 chemical sciences, law.invention, Resonant inelastic X-ray scattering, chemistry.chemical_compound, Ferrocene, chemistry, Beamline, law, 0103 physical sciences, Emission spectrum, Atomic physics, 010306 general physics, Instrumentation, ComputingMilieux_MISCELLANEOUS, Astrophysics::Galaxy Astrophysics, Emission Spectrometer, Group 2 organometallic chemistry
Abstract

A new setup has been designed and built to study organometallic complexes in gas phase at the third-generation Synchrotron radiation sources. This setup consists of a new homemade computer-controlled gas cell that allows us to sublimate solid samples by accurately controlling the temperature. This cell has been developed to be a part of the high-resolution X-ray emission spectrometer permanently installed at the GALAXIES beamline of the French National Synchrotron Facility SOLEIL. To illustrate the capabilities of the setup, the cell has been successfully used to record high-resolution Kα emission spectra of gas-phase ferrocene Fe(C5H5)2 and to characterize their dependence with the excitation energy. This will allow to extend resonant X-ray emission to different organometallic molecules.

Published
2018

43. Resonant inelastic X-ray spectroscopy of atoms and simple molecules: Satellite features and dependence on energy detuning and photon polarization

Author

Renaud Guillemin, E. Kawerk, Klemen Bučar, Marc Simon, L. Journel, Tatiana Marchenko, A. Mihelič, Maria Novella Piancastelli, Wei Cao, R. Bohinc, M. Kavčič, Stéphane Carniato, Matjaž Žitnik, Jozef Stefan Institute [Ljubljana] (IJS), Department of Physics [Hong Kong University of Science and Technology], Hong Kong University of Science and Technology (HKUST), RIKEN - Institute of Physical and Chemical Research [Japon] (RIKEN), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire pour l'utilisation du rayonnement électromagnétique (LURE), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-MENRT-Centre National de la Recherche Scientifique (CNRS)

Subjects
Photon, Astrophysics::High Energy Astrophysical Phenomena, 02 engineering and technology, Electron, 01 natural sciences, Electromagnetic radiation, 0103 physical sciences, Photon polarization, [CHIM]Chemical Sciences, Physical and Theoretical Chemistry, 010306 general physics, Spectroscopy, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], X-ray spectroscopy, Radiation, Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Polarization (waves), Atomic and Molecular Physics, and Optics, Electronic, Optical and Magnetic Materials, Excited state, Atomic physics, 0210 nano-technology
Abstract

We summarize recent results dealing with high resolution (resonant) X-ray spectroscopy of atomic and molecular targets in the tender X-ray energy region. We comment on advantages, new possibilities and problems related to RIXS spectroscopy with respect to the standard photoabsorption technique, where scanning the probe energy is the only option. In particular, three research areas are covered: X-ray emission mediated by energy dependent photoabsorption to multi-electron excited states, the Cl K core-hole clock studies exemplified by systematic study of chloro(fluoro)-hydrocarbon targets and the polarization dependent X-ray emission studies. Due to its spectral selectivity and simultaneous detection capability, high resolution wavelength dispersive X-ray spectroscopy has the capability to resolve structural and dynamical properties of matter within new instrumentation frontiers.

Published
2015

44. Electron dynamics in the core-excited CS 2 molecule revealed through resonant inelastic x-ray scattering spectroscopy

Author

Renaud Guillemin, L. Journel, E. Kawerk, R. Bohinc, Marielle Simon, Vinícius Vaz da Cruz, Klemen Bučar, M. Kavčič, Faris Gel'mukhanov, Matjaž Žitnik, Stéphane Carniato, Tatiana Marchenko, Marko Petric, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), School of Biotechnology [Stockholm], Jozef Stefan Institute [Ljubljana] (IJS), Theoretical Chemistry and Biology [Stockholm], Université Libanaise, Royal Institute of Biotechnology (KTH), Synchrotron SOLEIL (SSOLEIL), and Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], History, Scattering, Chemistry, Dephasing, Physics, QC1-999, 02 engineering and technology, Inelastic scattering, 021001 nanoscience & nanotechnology, 01 natural sciences, Resonance (particle physics), Molecular physics, Computer Science Applications, Education, Resonant inelastic X-ray scattering, Excited state, 0103 physical sciences, Condensed Matter::Strongly Correlated Electrons, Atomic physics, 010306 general physics, 0210 nano-technology, Spectroscopy, Excitation
Abstract

International audience; We present an experimental and theoretical study of resonant inelastic x-ray scattering (RIXS) in the carbon disulphide CS 2 molecule near the sulfur K-absorption edge. We observe a strong evolution of the RIXS spectral profile with the excitation energy tuned below the lowest unoccupied molecular orbital (LUMO) absorption resonance. The reason for this is twofold. Reducing the photon energy in the vicinity of the LUMO absorption resonance leads to a relative suppression of the LUMO contribution with respect to the emission signal from the higher unoccupied molecular orbitals, which results in the modulation of the total RIXS profile. At even larger negative photon-energy detuning from the resonance, the excitation-energy dependence of the RIXS profile is dominated by the onset of electron dynamics triggered by a coherent excitation of multiple electronic states. Furthermore, our study demonstrates that in the hard x-ray regime, localization of the S 1s core hole occurs in CS 2 during the RIXS process because of the orientational dephasing of interference between the waves scattering on the two sulfur atoms. Core-hole localization leads to violation of the symmetry selection rules for the electron transitions observed in the spectra.

Published
2015

45. Ultrafast Dynamics And Electronic State – Lifetime Interferences In Chlorine-Containing Molecules

Author

L. Journel, R. K. Kushawaha, Gildas Goldsztejn, Denis Céolin, Renaud Guillemin, Marielle Simon, Maria Novella Piancastelli, Tatiana Marchenko, Ralph Püttner, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Pierre et Marie Curie - Paris 6 (UPMC), Institut für Experimentalphysik, Freie Universität Berlin, Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Department of Physics and Astronomy [Uppsala], Uppsala University, and Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
History, Photon, 010304 chemical physics, Chemistry, Electronic structure, 7. Clean energy, 01 natural sciences, Resonance (particle physics), Spectral line, Synchrotron, Computer Science Applications, Education, law.invention, Beamline, law, Excited state, 0103 physical sciences, Physical Sciences, Fysik, Atomic physics, 010306 general physics, [PHYS.ASTR]Physics [physics]/Astrophysics [astro-ph], Ultrashort pulse
Abstract

International audience; In order to have access to fine phenomena such as ultrafast nuclear dynamics and electronic state - lifetime interferences (ELI) at high energies (few keV), one has to rely on great experimental resolution. The new experimental HAXPES endstation at the GALAXIES beamline of the French synchrotron SOLEIL provides photons in the 2-12 keV energy range along with a total instrumental resolution below 500 meV. In this work we show experimental evidences of ultrafast nuclear dynamics and ELI on HCl and CH3Cl excited around the Cl 1s resonance. We show also simulations that allow to disentangle the contribution of nuclear dynamics and ELI in our experimental spectra.

Published
2015

46. Double core-hole states in SiX4 (X = F, Cl, Br, and CH3) molecules derived by photoelectron and KLL Auger spectroscopy

Author

Maria Novella Piancastelli, Tatiana Marchenko, Ralph Püttner, Marielle Simon, Renaud Guillemin, Gildas Goldsztejn, Kiyoshi Ueda, Dennis W. Lindle, L. Journel, Osamu Takahashi, D Céolin, J-P Rueff, Alexsandre F. Lago, Institut für Experimentalphysik, Freie Universität Berlin, Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), University of Nevada [Las Vegas] (WGU Nevada), Centro de Ciências Naturais e Humanas, Universidade Federal do ABC (UFABC), Institute of Multidisciplinary Research for Advanced Materials, Tohoku University [Sendai], Department of Chemistry [Hiroshima], Department of Physics and Astronomy [Uppsala], Uppsala University, and Universidade Federal do ABC = Federal University of ABC = Université Fédérale de l'ABC [Brazil] (UFABC)

Subjects
[PHYS]Physics [physics], History, Auger electron spectroscopy, 010304 chemical physics, Chemistry, Chemical shift, Binding energy, 01 natural sciences, Electron spectroscopy, 3. Good health, Computer Science Applications, Education, X-ray photoelectron spectroscopy, 0103 physical sciences, Physical Sciences, Relaxation (physics), Molecule, Fysik, Atomic physics, 010306 general physics, Spectroscopy
Abstract

International audience; In recent years double core-hole states are intensively studied since their chemical shifts provide detailed information about initial-state and relaxation effects in a molecule. We derived the Si 1s−1, 2s−1, and 2p−1 binding energies as well as the Si 2s−2, 2s−1, 2p−1, and 2p−2 double-core hole binding energies of different SiX4 systems in order to derive the chemical shifts. Based on these results we created Wagner plots, which give insight in the initial state and the relaxation effects in the different molecules.

Published
2015

47. New achievements on relaxation dynamics of atoms and molecules photoexcited in the tender x-ray domain at synchrotron SOLEIL

Author

Renaud Guillemin, Maria Novella Piancastelli, T. Marin, Marc Simon, Gildas Goldsztejn, Oksana Travnikova, L. Journel, B. Cunha de Miranda, I. Ismail, and Tatiana Marchenko

Subjects
Physics, Photon, Astrophysics::High Energy Astrophysical Phenomena, Atoms in molecules, X-ray, 02 engineering and technology, Electron, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, Crystallographic defect, Atomic and Molecular Physics, and Optics, Charged particle, Synchrotron, law.invention, law, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Atomic physics, 010306 general physics, 0210 nano-technology, Spectroscopy
Abstract

The so-called 'tender' x-ray domain, from 2 to 13 keV, has recently become available for atomic and molecular studies at the French synchrotron SOLEIL with state-of-the-art photon and electron ener ...

Published
2017

48. Coulomb explosion of diatomic molecules in intense XUV fields mapped by partial covariance

Author

D.M.P. Holland, S. Düsterer, Marcus Rosenblatt, K. Motomura, Kiyoshi Ueda, Per Johnsson, M. Siano, Arnaud Rouzée, Leszek J. Frasinski, Oleg Kornilov, A. Lübcke, Tatiana Marchenko, Claus-Peter Schulz, Martin Eckstein, F Schapper, Lutz Foucar, Thomas Schlathölter, Marc J. J. Vrakking, J. Klei, and Research unit Astroparticle Physics

Subjects
COINCIDENCE, Covariance mapping, SPATIAL ALIGNMENT, 02 engineering and technology, Kinetic energy, 01 natural sciences, 7. Clean energy, Spectral line, FREE-ELECTRON LASER, Ionization, 0103 physical sciences, ddc:530, ION, EXTREME-ULTRAVIOLET, 010306 general physics, Physics, MICROCHANNEL PLATES, Coulomb explosion, VELOCITY, Covariance, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Diatomic molecule, Atomic and Molecular Physics, and Optics, PULSES, IONIZATION, Atomic physics, 0210 nano-technology, Ground state, X-RAY LASER
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.

Published
2013

49. Scaling laws for photoelectron holography in the midinfrared wavelength regime

Author

Y. Huismans, Giel Berden, Arnaud Rouzée, Joost M. Bakker, A. Gijsbertsen, A.F.G. van der Meer, P S W M Logman, Franck Lépine, Tatiana Marchenko, Cécile Cauchy, Britta Redlich, Tian-Min Yan, Julia H. Jungmann, M. Yu. Ivanov, Aneta Smolkowska, Olga Smirnova, Dieter Bauer, Sébastien Zamith, Marc J. J. Vrakking, FOM Institute for Atomic and Molecular Physics (AMOLF), Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), Laboratoire de Spectrométrie Ionique et Moléculaire (LASIM), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Agrégats (LCAR), Laboratoire Collisions Agrégats Réactivité (LCAR), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), FOM Institute for Plasma Physics, FOM, Department of Physics [Imperial College London], Imperial College London, Max-Planck-Institut für Kernphysik (MPIK), Max-Planck-Gesellschaft, Institut für Physik, Universität Rostock, Universität Rostock, Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Chemistry and Pharmaceutical Sciences, Research and Theory in Education, VU SBE Executive Education, and Physical Chemistry

Subjects
Materials science, Holography, General Physics and Astronomy, chemistry.chemical_element, Physics::Optics, 01 natural sciences, law.invention, Ion, 010309 optics, Xenon, law, Metastability, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, 010306 general physics, GeneralLiterature_REFERENCE(e.g.,dictionaries,encyclopedias,glossaries), 32.80.Rm, 32.80.Wr, Molecular Structure and Dynamics, [PHYS.PHYS.PHYS-ATOM-PH]Physics [physics]/Physics [physics]/Atomic Physics [physics.atom-ph], Molecular and Biophysics, Free-electron laser, Laser, Wavelength, chemistry, Atomic physics
Abstract

International audience; Midinfrared strong-field laser ionization offers the promise of measuring holograms of atoms and molecules, which contain both spatial and temporal information of the ion and the photoelectron with subfemtosecond temporal and angstrom spatial resolution. We report on the scaling of photoelectron holographic interference patterns with the laser pulse duration, wavelength, and intensity. High-resolution holograms for the ionization of metastable xenon atoms by 7-16 m light from the FELICE free electron laser are presented and compared to semiclassical calculations that provide analytical insight.

Published
2012

50. Time-resolved holography with photoelectrons

Author

Olga Smirnova, Dieter Bauer, Franck Lépine, Marcus Vrakking, C. Cauchy, Britta Redlich, Harm Geert Muller, Julia H. Jungmann, Sébastien Zamith, M. Yu. Ivanov, Kenneth J. Schafer, Tatiana Marchenko, Joost M. Bakker, A. Gijsbertsen, Y. Huismans, Giel Berden, P S W M Logman, S. V. Popruzhenko, Arnaud Rouzée, A.F.G. van der Meer, Aneta Smolkowska, W Vermin, Michael Spanner, FOM Institute for Atomic and Molecular Physics (AMOLF), Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI), Laboratoire de Spectrométrie Ionique et Moléculaire (LASIM), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Agrégats (LCAR), Laboratoire Collisions Agrégats Réactivité (LCAR), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université de Toulouse (UT)-Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Chimie Physique - Matière et Rayonnement (LCPMR), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), FOM Institute for Plasma Physics, FOM, Computing and Networking Services (SARA), Department of Physics and Astronomy [Baton Rouge], Louisiana State University (LSU), National Research Council of Canada (NRC), Department of Physics [Imperial College London], Imperial College London, Institut für Physik, Universität Rostock, Universität Rostock, Moscow Engineering Physics Institute, The National Research Nuclear University MEPhI (Moscow Engineering Physics Institute) [Moscow, Russia], Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées, Chemistry and Pharmaceutical Sciences, Research and Theory in Education, VU SBE Executive Education, Physics and Astronomy, Physical Chemistry, Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)

Subjects
Attosecond, Holography, chemistry.chemical_element, Physics::Optics, Photoionization, 7. Clean energy, 01 natural sciences, 010305 fluids & plasmas, law.invention, Xenon, Optics, law, Ionization, 0103 physical sciences, Physics::Atomic and Molecular Clusters, Physics::Atomic Physics, 010306 general physics, Multidisciplinary, Molecular Structure and Dynamics, business.industry, Molecular and Biophysics, Atoms in molecules, [PHYS.PHYS.PHYS-ATM-PH]Physics [physics]/Physics [physics]/Atomic and Molecular Clusters [physics.atm-clus], Photoelectric effect, Laser, chemistry, Atomic physics, business
Abstract

International audience; Ionization is the dominant response of atoms and molecules to intense laser fields and is at the basis of several important techniques, such as the generation of attosecond pulses that allow the measurement of electron motion in real time. We present experiments in which metastable xenon atoms were ionized with intense 7-micrometer laser pulses from a free-electron laser. Holographic structures were observed that record underlying electron dynamics on a sublaser-cycle time scale, enabling photoelectron spectroscopy with a time resolution of almost two orders of magnitude higher than the duration of the ionizing pulse.

Published
2011

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