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

Inhester, Ludger; Hanasaki, Kota; Hao, Yajiang; Son, Sang−Kil; Santra, Robin

doi:10.1103/physreva.94.023422

Cited by 43 publications

(72 citation statements)

References 49 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Every K-shell ionization is accompanied by the corresponding relaxation of the core hole, i.e., Auger decay or x-ray fluorescence. As has been described before [35], we model this ionization dynamics using the coupled rate equations,…”

Section: Methodsmentioning

confidence: 99%

“…In molecules, the radiation damage can be significantly different from what one would expect for single atoms [35,36]. Here we analyze how the complex ionization dynamics at high x-ray intensity involving various different charge states manifests itself in the molecular photoelectron, Auger electron, and fluorescence spectra.…”

Section: Introductionmentioning

confidence: 98%

“…Here we analyze how the complex ionization dynamics at high x-ray intensity involving various different charge states manifests itself in the molecular photoelectron, Auger electron, and fluorescence spectra. We employ our x-ray molecular physics toolkit XMOLECULE [35,37] to calculate various spectra for a molecule exposed to an intense x-ray pulse. We choose a water molecule as a test system.…”

Section: Introductionmentioning

confidence: 99%

“…We choose a water molecule as a test system. In our approach [35] the time-dependent population of the electronic configurations is described with a rate equation model. For comparable applications of rate equations see Refs.…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

et al. 2018

Self Cite

View full text Add to dashboard Cite

With the highly intense x-ray light generated by x-ray free-electron lasers (XFELs), molecular samples can be ionized many times in a single pulse. Here we report on a computational study of molecular spectroscopy at the high x-ray intensity provided by XFELs. Calculated photoelectron, Auger electron, and x-ray fluorescence spectra are presented for a single water molecule that reaches many electronic hole configurations through repeated ionization steps. The rich details shown in the spectra depend on the x-ray pulse parameters in a nonintuitive way. We discuss how the observed trends can be explained by the competition of microscopic electronic transition processes. A detailed comparison between spectra calculated within the independent-atom model and within the molecular-orbital framework highlights the chemical sensitivity of the spectral lines of multiple-hole configurations. Our results demonstrate how x-ray multiphoton ionization-related effects such as charge-rearrangement-enhanced x-ray ionization of molecules and frustrated absorption manifest themselves in the electron and fluorescence spectra.

show abstract

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

et al. 2018

Self Cite

View full text Add to dashboard Cite

show abstract

“…The atomic electronic structure and atomic data calculated by xatom have served as inputs to xmdyn to simulate complex systems such as C 60 [46] and Ar and Xe clusters [47] interacting with intense XFEL pulses. They have also been used for xmolecule to calculate molecular electronic structure [59] and molecular data [60] to investigate molecular x-ray multiphoton ionization dynamics [60] and ultrafast explosion dynamics of small polyatomic molecules induced by intense XFEL pulses [61]. Lastly, xatom has been extended to treat atoms and ions immersed in a plasma environment to investigate ionization potential lowering in warm dense matter [62,63], which has further been employed for studying x-ray resonant magnetic scattering in materials [64].…”

Section: Introductionmentioning

confidence: 99%

Compton spectra of atoms at high x-ray intensity

Son

Geffert

Santra

2017

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

Self Cite

View full text Add to dashboard Cite

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.

show abstract

Dissociating diatomic molecules in ultrafast and intense light

Buth

2019

Chemical Physics

View full text Add to dashboard Cite

An ab initio theory is devised for the quantum dynamics of molecules undergoing (multiple) ionization in ultrafast and intense light. Specifically, the intertwined problem of photoionization, radiative, and electronic transitions in the course of dissociation is addressed which arises, e.g., when molecules are exposed to xuv light or x rays from free electron lasers or attosecond light sources, but the approach is equally useful in optical strong-field physics. The coherent interaction of the molecule with the light in a specific charge state is also treated. I set out from an abstract formulation in terms of the quantum optical notion of system-reservoir interaction using a master equation in Lindblad form and analyze its short-time approximation. First, I express it in a direct sum rigged Hilbert space for an efficient solution with numerical methods for systems of differential equations. Second, I derive a treatment via quantum Monte Carlo wave packet (MCWP) propagation. The formalism is concretized to diatomic molecules in Born-Oppenheimer approximation whereby molecular rotation is disregarded. The numerical integration of the master equation is carried out with a suitably factored density matrix that exploits the locality of the Hamiltonian and the Lindblad superoperator with respect to the internuclear distance. The formulation of the MCWP for molecules requires a thorough analysis of the quantum jump process; namely, the dependence on the continuous distance renders a straight wave packet promotion useless and, instead, a projected outer product needs to be employed involving an integrated quantum jump operator.

show abstract

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

Cited by 43 publications

References 49 publications

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

Electron and fluorescence spectra of a water molecule irradiated by an x-ray free-electron laser pulse

Compton spectra of atoms at high x-ray intensity

Dissociating diatomic molecules in ultrafast and intense light

Contact Info

Product

Resources

About