Auger Electron Angular Distribution of Double Core-Hole States in the Molecular Reference Frame

PostprintThis is the accepted version of a paper published in Chemical Physics Letters. This paper has been peerreviewed but does not include the final publisher proof-corrections or journal pagination.Citation for the original published paper (version of record):Eland, J H., Linusson, P., Mucke, M., Feifel, R. (2012) Homonuclear site-specific photochemistry by an ion-electron multi-coincidence spectroscopy technique. Abstract By combining multi-particle coincidence detection of electrons and ions with ionization by soft X-ray synchrotron radiation we demonstrate an effective tool for atomic spectroscopy and sitespecific photochemistry. Its most novel capability is application to molecular fragmentation after K-shell vacancy production in atoms distinguished only by their chemical environment. Chemical Physics Letters

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“…Refs. [22][23][24][25][26] and references therein) than for single holes, and to be especially strong for two-site double core holes (cf. Refs.…”

Section: Introductionmentioning

confidence: 99%

Homonuclear site-specific photochemistry by an ion–electron multi-coincidence spectroscopy technique

Eland

Linusson

Mucke

et al. 2012

Chemical Physics Letters

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“…They suggested (4) that intense, ultrashort pulses could allow such investigations via a nonlinear two-photon absorption process. Such experimental observations were not possible until the recent (6, 7) advent of ultrafast X-ray free-electron lasers (FELs), which are revolutionizing spectroscopy (8)(9)(10)(11)(12) and imaging (13).…”

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confidence: 99%

Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser

Berrah

Murphy

et al. 2011

Proc. Natl. Acad. Sci. U.S.A.

177

130

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Theory predicts that double-core-hole (DCH) spectroscopy can provide a new powerful means of differentiating between similar chemical systems with a sensitivity not hitherto possible. Although DCH ionization on a single site in molecules was recently measured with double-and single-photon absorption, double-core holes with single vacancies on two different sites, allowing unambiguous chemical analysis, have remained elusive. Here we report that direct observation of double-core holes with single vacancies on two different sites produced via sequential two-photon absorption, using short, intense X-ray pulses from the Linac Coherent Light Source free-electron laser and compare it with theoretical modeling. The observation of DCH states, which exhibit a unique signature, and agreement with theory proves the feasibility of the method. Our findings exploit the ultrashort pulse duration of the free-electron laser to eject two core electrons on a time scale comparable to that of Auger decay and demonstrate possible future X-ray control of physical inner-shell processes.multi-photon ionization | ultrafast | two-photon spectroscopy

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“…Specifically, we demonstrate the effects of high per-atom X-ray absorption on the fragmentation dynamics of C 60 molecules in the gas phase. C 60 offers a number of advantages as a benchmark molecule when compared with isolated atoms [29][30][31][32][33] , small molecules [34][35][36][37][38][39][40] or van der Waals (vdW) clusters 41,42 , from the perspective of radiation damage. C 60 consists of chemically bonded carbon atoms with representative bond lengths and damage processes.…”

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confidence: 99%

Femtosecond X-ray-induced explosion of C60 at extreme intensity

et al. 2014

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Understanding molecular femtosecond dynamics under intense X-ray exposure is critical to progress in biomolecular imaging and matter under extreme conditions. Imaging viruses and proteins at an atomic spatial scale and on the time scale of atomic motion requires rigorous, quantitative understanding of dynamical effects of intense X-ray exposure. Here we present an experimental and theoretical study of C 60 molecules interacting with intense X-ray pulses from a free-electron laser, revealing the influence of processes not previously reported. Our work illustrates the successful use of classical mechanics to describe all moving particles in C 60 , an approach that scales well to larger systems, for example, biomolecules. Comparisons of the model with experimental data on C 60 ion fragmentation show excellent agreement under a variety of laser conditions. The results indicate that this modelling is applicable for X-ray interactions with any extended system, even at higher X-ray dose rates expected with future light sources.

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Auger Electron Angular Distribution of Double Core-Hole States in the Molecular Reference Frame

Cited by 171 publications

References 27 publications

Homonuclear site-specific photochemistry by an ion–electron multi-coincidence spectroscopy technique

Homonuclear site-specific photochemistry by an ion–electron multi-coincidence spectroscopy technique

Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser

Femtosecond X-ray-induced explosion of C60 at extreme intensity

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