Double core-hole formation in small molecules at the LCLS free electron laser

Larsson, Mats; Salén, Peter; Meulen, P. van der; Schmidt, H. T.; Thomas, Richard; Feifel, Raimund; Piancastelli, Maria Novella; Li, Fang; Murphy, Brendan; Osipov, T.; Berrah, N.; Kukk, E.; Ueda, Kiyoshi; Bozek, John D.; Bostedt, Christoph; Wada, S.; Richter, Robert; Feyer, Vitaliy

doi:10.1088/0953-4075/46/16/164030

Cited by 19 publications

(18 citation statements)

References 40 publications

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“…and |χ S DCH ij ( k, k , t) are the nuclear wave packets associated with the ground, the SCH and the DCH states, respectively. Satellite states are not considered in the present work even if they can be found in the same energy region as DCH resonances [10,13,36], because they can be circumvented by measuring in coincidence the two photoelectrons.…”

Section: A Equations Of Motionmentioning

confidence: 99%

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Time-dependent quantum description of molecular double-core-hole-state formation: Impact of the nuclear dynamics on sequential two-photon processes

et al. 2018

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We present a theoretical model to investigate double core hole states formation in molecules through sequential absorption of two x-ray photons from a femtosecond laser pulse. A complete time-dependent quantum description taking into account x-ray absorption and nuclear dynamics explicitly and Auger decay phenomenologically is established within the local approximation. Using this model, we assess the impact of the nuclear dynamics on double core photoionization processes in the case of the carbon monoxide molecule. We show that sequential absorption of two x-ray photons modifies significantly the vibrational distribution of the photoelectron spectra of the double core hole states compared to direct single x-ray photon absorption. Depending on the shape of the potential energy curves involved in the sequential absorption processes, lower or higher vibrational levels may be favoured. Furthermore, in case the final state is dissociative, the electron spectrum is further broaden and blue-shifted in the two-photon process.

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Section: A Equations Of Motionmentioning

confidence: 99%

“…Due to the very recent development of XFELs, only few observations of DCH states have been carried out. Most investigations concern atoms [2,[5][6][7][8][9], or multiply core ionized small molecules [10][11][12][13][14][15][16].…”

Section: Introductionmentioning

confidence: 99%

Time-dependent quantum description of molecular double-core-hole-state formation: Impact of the nuclear dynamics on sequential two-photon processes

et al. 2018

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“…Double-core hole states have recently been experimentally realized in the gas phase [57,75]. Creation of double-core hole states in water should hence be possible with the intensities available at XFELs and pulses of a few femtoseconds.…”

Section: High Fluence Effects and Nonlinear X-ray Spectroscopy In Watermentioning

confidence: 99%

Probing water with X-ray lasers

Nilsson

Schreck

Perakis

et al. 2016

Advances in Physics: X

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Here, we discuss three cases where the X-ray free-electron laser, the Linac Coherent Light Source, has been used to probe water. The ability to cool water very rapidly down to 227 K and to probe it with ultrashort (50 fs) X-ray pulses before freezing has allowed for investigating water structure below the previous limit of homogeneous ice nucleation. It was found that at the temperature where the thermodynamic response functions, such as heat capacity and isothermal compressibility, seem to diverge there is no discontinuous change in structure, but instead an accelerated transformation from a disordered state to a strongly tetrahedral. The ice nucleation rate in bulk-like micron-sized water droplets could be determined for temperatures down to 227 K and was shown to be ~8 orders of magnitude lower than previous data for nanodroplets. The application to X-ray spectroscopy is discussed based on measurements at high X-ray fluence where multiple valence-hole states can be generated. Finally, a perspective to the future is presented regarding X-ray photon correlation spectroscopy with which true equilibrium dynamical properties can be studied.

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“…It has shown that it has greater potential to probe the local chemical environment than by detecting single corehole (SCH) spectroscopy. Secondly, combining with accurate theoretical simulations [14], DCH spectroscopy provides a useful tool for estimating or even diagnosing the intensity and duration of x-ray pulses [15]. In dense plasmas, it reflects the screening effects on atoms embedded in the plasmas produced by x-ray laser pulses [16,17,18,19] and thus it can be utilized to deduce the environmental effects.…”

Section: Introductionmentioning

confidence: 99%

Single- and double-core-hole ion emission spectroscopy of transient neon plasmas produced by ultraintense x-ray laser pulses

Cheng

Zeng

Yuan

2016

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

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Double core-hole (DCH) spectroscopy is investigated systematically for neon atomic system in the interaction with ultraintense x-ray pulses with photon energy from 937 eV to 2000 eV. A time-dependent rate equation, implemented in the detailed level accounting approximation, is utilized to study the dynamical evolution of the level population and emission properties of the highly transient plasmas. For x-ray pulses with photon energy in the range of 937-1030 eV, where 1s → 2p resonance absorption from single core-hole (SCH) states of neon charge states exist, inner-shell resonant absorption (IRA) effects play important roles in the time evolution of population and DCH spectroscopy. Such IRA physical effects are illustrated in detail by investigating the interaction of x-ray pulses at a photon energy of 944 eV, which corresponds to the 1s → 2p resonant absorption from the SCH states (1s2s 2 2p 4 , 1s2s2p 5 and 1s2p 6 ) of Ne 3+ . After averaging over the space and time distribution of the x-ray pulses, DCH spectroscopy at photon energies of 937, 944, 955, 968, 980, and 990 eV (corresponding to the 1s → 2p resonance energies of Ne 2+ -Ne 7+ , respectively) are studied in detail. The complex mechanisms of producing the DCH states are discussed, taking the DCH spectroscopy at 937 and 980 eV as examples. For photon energy larger than 1362 eV, there are no resonance absorption in the interaction, resulting in a similar physical picture of DCH spectroscopy. The dominant DCH states are due to higher ionization stages of Ne 7+ -Ne 9+ , while the DCH spectroscopy from lower charge states Ne 2+ -Ne 6+ are much weaker. With the increase of x-ray photon energy, the contributions from the lower charge states become larger.

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Double core-hole formation in small molecules at the LCLS free electron laser

Abstract: Introduction

Cited by 19 publications

References 40 publications

Time-dependent quantum description of molecular double-core-hole-state formation: Impact of the nuclear dynamics on sequential two-photon processes

Time-dependent quantum description of molecular double-core-hole-state formation: Impact of the nuclear dynamics on sequential two-photon processes

Probing water with X-ray lasers

Single- and double-core-hole ion emission spectroscopy of transient neon plasmas produced by ultraintense x-ray laser pulses

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