TY - JOUR A1 - Berrah, N. A1 - Sánchez-González, Álvaro A1 - Jurek, Zoltan A1 - Obaid, Razib A1 - Xiong, H. A1 - Squibb, R. J. A1 - Osipov, T. A1 - Lutman, A. A1 - Fang, L. A1 - Barillot, T. A1 - Bozek, J. D. A1 - Cryan, J. A1 - Wolf, T. J. A. A1 - Rolles, Daniel A1 - Coffee, R. A1 - Schnorr, Kirsten A1 - Augustin, S. A1 - Fukuzawa, Hironobu A1 - Motomura, K. A1 - Niebuhr, Nina Isabelle A1 - Frasinski, L. J. A1 - Feifel, Raimund A1 - Schulz, Claus-Peter A1 - Toyota, Kenji A1 - Son, Sang-Kil A1 - Ueda, K. A1 - Pfeifer, T. A1 - Marangos, J. P. A1 - Santra, Robin T1 - Femtosecond-resolved observation of the fragmentation of buckminsterfullerene following X-ray multiphoton ionization JF - Nature physics N2 - X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C-60), exposed to 640 eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20 fs) X-ray pump pulse, the fragmentation of C-60 is considerably delayed. This work uncovers the persistence of the molecular structure of C-60, which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules. Y1 - 2019 U6 - https://doi.org/10.1038/s41567-019-0665-7 SN - 1745-2473 SN - 1745-2481 VL - 15 IS - 12 SP - 1279 EP - 1301 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Young, Linda A1 - Ueda, Kiyoshi A1 - Gühr, Markus A1 - Bucksbaum, Philip H. A1 - Simon, Marc A1 - Mukamel, Shaul A1 - Rohringer, Nina A1 - Prince, Kevin C. A1 - Masciovecchio, Claudio A1 - Meyer, Michael A1 - Rudenko, Artem A1 - Rolles, Daniel A1 - Bostedt, Christoph A1 - Fuchs, Matthias A1 - Reis, David A. A1 - Santra, Robin A1 - Kapteyn, Henry A1 - Murnane, Margaret A1 - Ibrahim, Heide A1 - Legare, Francois A1 - Vrakking, Marc A1 - Isinger, Marcus A1 - Kroon, David A1 - Gisselbrecht, Mathieu A1 - Wörner, Hans Jakob A1 - Leone, Stephen R. T1 - Roadmap of ultrafast x-ray atomic and molecular physics JF - Journal of physics : B, Atomic, molecular and optical physics N2 - X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (10(20) W cm(-2)) of x-rays at wavelengths down to similar to 1 Angstrom, and HHG provides unprecedented time resolution (similar to 50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of similar to 280 eV (44 Angstroms) and the bond length in methane of similar to 1 Angstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Angstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Angstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science. KW - ultrafast molecular dynamics KW - x-ray spectroscopies and phenomena KW - table-top sources KW - x-ray free-electron lasers KW - attosecond phenomena Y1 - 2018 U6 - https://doi.org/10.1088/1361-6455/aa9735 SN - 0953-4075 SN - 1361-6455 VL - 51 IS - 3 PB - IOP Publ. Ltd. CY - Bristol ER - TY - GEN A1 - Young, Linda A1 - Ueda, Kiyoshi A1 - Gühr, Markus A1 - Bucksbaum, Philip H. A1 - Simon, Marc A1 - Mukamel, Shaul A1 - Rohringer, Nina A1 - Prince, Kevin C. A1 - Masciovecchio, Claudio A1 - Meyer, Michael A1 - Rudenko, Artem A1 - Rolles, Daniel A1 - Bostedt, Christoph A1 - Fuchs, Matthias A1 - Reis, David A. A1 - Santra, Robin A1 - Kapteyn, Henry A1 - Murnane, Margaret A1 - Ibrahim, Heide A1 - Légaré, François A1 - Vrakking, Marc A1 - Isinger, Marcus A1 - Kroon, David A1 - Gisselbrecht, Mathieu A1 - L'Huillier, Anne A1 - Wörner, Hans Jakob A1 - Leone, Stephen R. T1 - Roadmap of ultrafast x-ray atomic and molecular physics T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm−2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 668 KW - ultrafast molecular dynamics KW - x-ray spectroscopies and phenomena KW - table-top sources KW - x-ray free-electron lasers KW - attosecond phenomena Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-424238 SN - 1866-8372 IS - 668 ER -