Evidence for interatomic Coulombic decay in Xe<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mi>K</mml:mi></mml:math>-shell-vacancy decay of XeF<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow /><mml:mn>2</mml:mn></mml:msub></mml:math>

Dunford, R. W.; Southworth, Stephen H.; Ray, D.; Kanter, E. P.; Krässig, B.; Young, Linda; Arms, D. A.; Đufresne, Eric M.; Walko, Donald A.; Vendrell, Oriol; Son, Sang−Kil; Santra, Robin

doi:10.1103/physreva.86.033401

Cited by 15 publications

(17 citation statements)

References 28 publications

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“…In a XeF 2 molecule, the dynamics triggered by the 3 d inner-shell hole relaxation is more interesting and rich. The charge is redistributed from the Xe site to the F sites, and the highly charged states of the molecule end up dissociating into three atomic ions 21 22 . In XeF 2 molecule, this results in a wide range of dissociating channels .…”

Section: Resultsmentioning

confidence: 99%

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

et al. 2016

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New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Particularly, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. Here we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF2 molecules following X-ray absorption at the Xe site.

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Section: Resultsmentioning

confidence: 99%

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

et al. 2016

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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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“…The x-ray multiphoton ionization model has been applied to study the impact of frustrated absorption on elastic x-ray scattering dynamics [48]. The dynamical information of multiple ionization has been employed to interpret an x-ray-induced fragmentation experiment on small molecules at low xray intensity [49]. The time-dependent atomic form factors obtained from xatom have been used to construct diffraction patterns of nanocrystals exposed to intense x-ray pulses [50].…”

Section: Introductionmentioning

confidence: 99%

Compton spectra of atoms at high x-ray intensity

Son

Geffert

Santra

2017

J. Phys. B: At. Mol. Opt. Phys.

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Abstract. Compton scattering is the nonresonant inelastic scattering of an xray photon by an electron and has been used to probe the electron momentum distribution in gas-phase and condensed-matter samples. In the low x-ray intensity regime, Compton scattering from atoms dominantly comes from bound electrons in neutral atoms, neglecting contributions from bound electrons in ions and free (ionized) electrons. In contrast, in the high x-ray intensity regime, the sample experiences severe ionization via x-ray multiphoton multiple ionization dynamics. Thus, it becomes necessary to take into account all the contributions to the Compton scattering signal when atoms are exposed to high-intensity x-ray pulses provided by x-ray free-electron lasers (XFELs). In this paper, we investigate the Compton spectra of atoms at high xray intensity, using an extension of the integrated x-ray atomic physics toolkit, xatom.As the x-ray fluence increases, there is a significant contribution from ionized electrons to the Compton spectra, which gives rise to strong deviations from the Compton spectra of neutral atoms. The present study provides not only understanding of the fundamental XFEL-matter interaction but also crucial information for single-particle imaging experiments, where Compton scattering is no longer negligible.

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Evidence for interatomic Coulombic decay in XeK-shell-vacancy decay of XeF2

Cited by 15 publications

References 28 publications

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

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

Compton spectra of atoms at high x-ray intensity

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