Ultrafast Charge Rearrangement and Nuclear Dynamics upon Inner-Shell Multiple Ionization of Small Polyatomic Molecules

Erk, Benjamin; Rolles, Daniel; Foucar, L.; Rudek, Benedikt; Epp, Sascha W.; Cryle, Max J.; Bostedt, Christoph; Schorb, Sebastian; Bozek, John D.; Rouzée, Arnaud; Hundertmark, Axel; Marchenko, T.; Simon, M.; Filsinger, Frank; Christensen, Lars Rune; De, Sankar; Trippel, Sebastian; Küpper, Jochen; Stapelfeldt, Henrik; Wada, S.; Ueda, Kiyoshi; Swiggers, Michele; Messerschmidt, Marc; Schröter, C. D.; Moshammer, R.; Schlichting, Ilme; Ullrich, J.; Rudenko, Artem

doi:10.1103/physrevlett.110.053003

Cited by 106 publications

(111 citation statements)

References 26 publications

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“…Studying the response of a single molecule composed of a small number of atoms to the XFEL pulse is perhaps the most rewarding, as various levels of theory and experimental methods inapplicable to larger systems may be applied. This was illustrated by Erk et al, who reported ionization and fragmentation of methylselenol (CH 3 SeH) molecules by intense (>10 17 W=cm 2 ) 5-fs long x-ray pulses of about 2 keV energy, using coincident ion momentum spectroscopy [30]. They reported a molecular expansion of about 50% within the first 5-10 fs.…”

Section: Introductionmentioning

confidence: 86%

Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

Nagaya¹,

Motomura²,

Kukk³

et al. 2016

Phys. Rev. X

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Section: Introductionmentioning

confidence: 86%

Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

Nagaya¹,

Motomura²,

Kukk³

et al. 2016

Phys. Rev. X

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“…In this context electronic transition rates, i.e., photoionization cross sections and decay rates, were derived from the values for individual atoms. However, it has been found that relevant aspects of the radiation damage in molecules must be understood rather from the molecular electronic structure [7,[19][20][21][22][23]. Specifically, a core ionization that is purely located on one atomic site may give rise to charging up at another atomic site of the molecule, so the charges are redistributed among neighboring atoms within the molecule.…”

Section: Introductionmentioning

confidence: 99%

X-ray multiphoton ionization dynamics of a water molecule irradiated by an x-ray free-electron laser pulse

et al. 2016

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We present a theoretical investigation of x-ray multiphoton ionization dynamics of polyatomic molecules, based on the rate equation model and molecular electronic structure calculations. An efficient numerical procedure is developed to calculate photoionization cross sections, Auger rates, and fluorescence rates for all possible electronic multiple-hole configurations of molecules. We investigate the charge-state distribution of a water molecule after interaction with an intense x-ray pulse and discuss its dependence on the fluence and the pulse duration of the x-ray beam. Our results demonstrate that a water molecule exposed to an intense x-ray pulse is more ionized than what would be expected within the independent-atom picture.

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“…Molecular ionization and fragmentation follow absorption of a single synchrotron x ray [33][34][35] or absorption of multiple x rays using XFEL radiation [36][37][38][39][40]. In the present experiment, we exploited the femtosecond time resolution of XFEL pulses, but the fluences of the pump and probe pulses were designed to observe singlephoton pump and single-photon probe events.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy

et al. 2016

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The capability of generating two intense, femtosecond x-ray pulses with a controlled time delay opens the possibility of performing time-resolved experiments for x-ray-induced phenomena. We have applied this capability to study the photoinduced dynamics in diatomic molecules. In molecules composed of low-Z elements, K-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wave packets of the transient two-valence-hole states continue evolving on the femtosecond time scale, leading either to separated atomic ions or long-lived quasibound states. By using an x-ray pump and an x-ray probe pulse tuned above the K-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N 2 with a molecular dynamics model that accounts for K-shell ionization, Auger decay, and the time evolution of the nuclear wave packets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasibound states.

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Ultrafast Charge Rearrangement and Nuclear Dynamics upon Inner-Shell Multiple Ionization of Small Polyatomic Molecules

Cited by 106 publications

References 26 publications

Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

Ultrafast Dynamics of a Nucleobase Analogue Illuminated by a Short Intense X-ray Free Electron Laser Pulse

X-ray multiphoton ionization dynamics of a water molecule irradiated by an x-ray free-electron laser pulse

Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy

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