Nuclear dynamics during the resonant Auger decay of water molecules

Eroms, Matthis; Vendrell, Oriol; Jungen, Martin; Meyer, Hans‐Dieter; Cederbaum, Lorenz S.

doi:10.1063/1.3117902

Cited by 25 publications

(35 citation statements)

References 38 publications

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“…Other approaches, which address effects of nuclear motion in a coherent way and, thereby, are able to address vibrational features of the spectrum, rely on pre-calculated potential energy surfaces. For examples, Eroms et al 24 used the multi-configurational time-dependent Hartree technique to propagate the nuclear wave packets for the resonant Auger spectrum of water. Bao et al 25 presented a calculation of the normal Auger spectrum of the oxygen molecule based on the Kramers-Heisenberg formula.…”

Section: Introductionmentioning

confidence: 99%

Auger spectrum of a water molecule after single and double core ionization

Inhester

Burmeister

Groenhof

et al. 2012

The Journal of Chemical Physics

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The high intensity of free electron lasers opens up the possibility to perform single-shot molecule scattering experiments. However, even for small molecules, radiation damage induced by absorption of high intense x-ray radiation is not yet fully understood. One of the striking effects which occurs under intense x-ray illumination is the creation of double core ionized molecules in considerable quantity. To provide insight into this process, we have studied the dynamics of water molecules in single and double core ionized states by means of electronic transition rate calculations and ab initio molecular dynamics (MD) simulations. From the MD trajectories, photoionization and Auger transition rates were computed based on electronic continuum wavefunctions obtained by explicit integration of the coupled radial Schrödinger equations. These rates served to solve the master equations for the populations of the relevant electronic states. To account for the nuclear dynamics during the core hole lifetime, the calculated electron emission spectra for different molecular geometries were incoherently accumulated according to the obtained time-dependent populations, thus neglecting possible interference effects between different decay pathways. We find that, in contrast to the single core ionized water molecule, the nuclear dynamics for the double core ionized water molecule during the core hole lifetime leaves a clear fingerprint in the resulting electron emission spectra. The lifetime of the double core ionized water was found to be significantly shorter than half of the single core hole lifetime.

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Section: Introductionmentioning

confidence: 99%

Auger spectrum of a water molecule after single and double core ionization

Inhester

Burmeister

Groenhof

et al. 2012

The Journal of Chemical Physics

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“…The equations are similar to the present ones, but have to be augmented by the impact of the exciting pulse exactly as it has already been done for a single decay in Refs. [12,13,16]. Most importantly, the theory developed here can also be generalized to the case of cascades in which the nuclear motion plays a relevant role (e.g., in molecules and clusters).…”

Section: Discussionmentioning

confidence: 92%

Linewidth and lifetime of atomic levels and the time evolution of spectra and coincidence spectra

et al. 2010

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The time-dependent theory of an atomic cascade decay process is discussed. We show that it is useful to measure the spectra of the emitted particles (electrons or photons) as a function of time and introduce time-dependent spectra and time-dependent coincidence spectra. The analysis reveals that there are several timescales involved in the atomic cascades and in the respective spectra. The work prepares the ground for the discussion of molecules, clusters, and solids, where the nuclear dynamics strongly participate in the cascade decay process making it much more complex.

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“…13,15 In order to reproduce the relative intensity of the three core-excited resonances, an appropriate ratio of the transition dipole moments has to be taken into account. In our simulations, we use the following ratio of the squared electronic transition dipole moments 76 d 4a 1 ,0 2 : d 2b 2 ,0 2 : d 2b 1 ,0 2 = 1 : 1.37 : 0.57.…”

Section: Resultsmentioning

confidence: 99%

A study of the water molecule using frequency control over nuclear dynamics in resonant X-ray scattering

Cruz

Ertan

Couto

et al. 2017

Phys. Chem. Chem. Phys.

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In this combined theoretical and experimental study we report a full analysis of the resonant inelastic X-ray scattering (RIXS) spectra of HO, DO and HDO. We demonstrate that electronically-elastic RIXS has an inherent capability to map the potential energy surface and to perform vibrational analysis of the electronic ground state in multimode systems. We show that the control and selection of vibrational excitation can be performed by tuning the X-ray frequency across core-excited molecular bands and that this is clearly reflected in the RIXS spectra. Using high level ab initio electronic structure and quantum nuclear wave packet calculations together with high resolution RIXS measurements, we discuss in detail the mode coupling, mode localization and anharmonicity in the studied systems.

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Nuclear dynamics during the resonant Auger decay of water molecules

Cited by 25 publications

References 38 publications

Auger spectrum of a water molecule after single and double core ionization

Auger spectrum of a water molecule after single and double core ionization

Linewidth and lifetime of atomic levels and the time evolution of spectra and coincidence spectra

A study of the water molecule using frequency control over nuclear dynamics in resonant X-ray scattering

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