Sequential multiphoton multiple ionization of atomic argon and xenon irradiated by x-ray free-electron laser pulses from SACLA

Motomura, K.; Fukuzawa, H.; S-K, Son; Mondal, Subhendu; Tachibana, Takehiko; Ito, Yuta; Kimura, M.; Nagaya, K.; Sakai, Tsukasa; Matsunami, K.; Wada, S.; Hayashita, H.; Kajikawa, J.; Xj, Liu; Feifel, Raimund; Johnsson, Per; Siano, M.; Kukk, E.; Rudek, Benedikt; Erk, Benjamin; Foucar, L.; Robert, E.; Miron, Catalin; Tono, Kensuke; Inubushi, Yuichi; Hatsui, Takaki; Yabashi, Makina; Yao, Makoto; Santra, Robin; Ueda, Kiyoshi

doi:10.1088/0953-4075/46/16/164024

Cited by 51 publications

(56 citation statements)

References 39 publications

(70 reference statements)

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“…With the unprecedentedly high fluence provided by XFELs, a sample may easily undergo these processes many times during an x-ray pulse, ejecting many electrons. These multiphoton multiple ionization dynamics can be understood as a sequence of consecutive photoionization and Auger decay processes, which has been verified by a series of gas-phase experiments of isolated atoms and molecules at LCLS and SACLA [6][7][8][9][10][11][12][13]. Eventually, for the molecular case, * ludger.inhester@cfel.de † kota.hanasaki@cfel.de ‡ haoyj@ustb.edu.cn § sangkil.son@cfel.de robin.santra@cfel.de the highly charged sample will start to dissociate by Coulomb explosion.…”

Section: Introductionmentioning

confidence: 68%

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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Section: Introductionmentioning

confidence: 68%

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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“…Multiphoton absorption occurs during the pulse and the charge is also further increased by Auger cascades, as demonstrated in the case of xenon-an atom with a very similar electronic structure [36,37]. The Auger cascades are also the most likely mechanism of transferring charge to the methyl group of the molecule.…”

Section: Iodomethanementioning

confidence: 95%

Molecular Dynamics of XFEL-Induced Photo-Dissociation, Revealed by Ion-Ion Coincidence Measurements

et al. 2017

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X-ray free electron lasers (XFELs) providing ultrashort intense pulses of X-rays have proven to be excellent tools to investigate the dynamics of radiation-induced dissociation and charge redistribution in molecules and nanoparticles. Coincidence techniques, in particular multi-ion time-of-flight (TOF) coincident experiments, can provide detailed information on the photoabsorption, charge generation, and Coulomb explosion events. Here we review several such recent experiments performed at the SPring-8 Angstrom Compact free electron LAser (SACLA) facility in Japan, with iodomethane, diiodomethane, and 5-iodouracil as targets. We demonstrate how to utilize the momentum-resolving capabilities of the ion TOF spectrometers to resolve and filter the coincidence data and extract various information essential in understanding the time evolution of the processes induced by the XFEL pulses.

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“…The straightforward sequential multiphoton ionization model has been solved with a rate-equation approach [11,12] and verified with a series of XFEL experiments on gas-phased atoms: light atoms such as Ne [11,13] and Ar [14], and heavy atoms such as Kr [15] and Xe [14,16,17]. For example, the calculated charge-state distribution (CSD) of Xe at 2 keV showed an excellent agreement with experimental data [16].…”

Section: Introductionmentioning

confidence: 94%

Interplay between relativistic energy corrections and resonant excitations in x-ray multiphoton ionization dynamics of Xe atoms

2017

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In this paper, we theoretically study x-ray multiphoton ionization dynamics of heavy atoms taking into account relativistic and resonance effects. When an atom is exposed to an intense x-ray pulse generated by an x-ray free-electron laser (XFEL), it is ionized to a highly charged ion via a sequence of single-photon ionization and accompanying relaxation processes, and its final charge state is limited by the last ionic state that can be ionized by a single-photon ionization. If x-ray multiphoton ionization involves deep inner-shell electrons in heavy atoms, energy shifts by relativistic effects play an important role in ionization dynamics, as pointed out in Phys. Rev. Lett. 110, 173005 (2013). On the other hand, if the x-ray beam has a broad energy bandwidth, the high-intensity x-ray pulse can drive resonant photoexcitations for a broad range of ionic states and ionize even beyond the direct one-photon ionization limit, as first proposed in Nat. Photon. 6, 858 (2012). To investigate both relativistic and resonance effects, we extend the XATOM toolkit to incorporate relativistic energy corrections and resonant excitations in x-ray multiphoton ionization dynamics calculations. Charge-state distributions are calculated for Xe atoms interacting with intense XFEL pulses at a photon energy of 1.5 keV and 5.5 keV, respectively. For both photon energies, we demonstrate that the role of resonant excitations in ionization dynamics is altered due to significant shifts of orbital energy levels by relativistic effects. Therefore, it is necessary to take into account both effects to accurately simulate multiphoton multiple ionization dynamics at high x-ray intensity.

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Sequential multiphoton multiple ionization of atomic argon and xenon irradiated by x-ray free-electron laser pulses from SACLA

Cited by 51 publications

References 39 publications

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

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

Molecular Dynamics of XFEL-Induced Photo-Dissociation, Revealed by Ion-Ion Coincidence Measurements

Interplay between relativistic energy corrections and resonant excitations in x-ray multiphoton ionization dynamics of Xe atoms

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