Violation of centrosymmetry in time-resolved coherent x-ray diffraction from rovibrational states of diatomic molecules

Shao, Hua‐Chieh; Starace, Anthony F.

doi:10.1103/physreva.99.033413

Cited by 3 publications

(1 citation statement)

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“…Noncentrosymmetric scattering patterns can be observed with a setup in between our parallel and perpendicular setups [21,41]. We note in passing that recently a different type of deviation from centrosymmetry has been predicted [42].…”

Section: Simulations and Discussionmentioning

confidence: 76%

Time-resolved x-ray scattering from impulsively aligned or oriented molecules

2020

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Impulsive laser excitation of molecules can create rotational wave packets that lead to transient alignment or orientation. We present a theoretical analysis of the signatures of post-pulse field-free time-dependent alignment and orientation of diatomic molecules in time-resolved nonresonant x-ray scattering. This shows that alignment and its time dependence due to the interference terms of the rotational wave packet are visible in the x-ray scattering signal whereas signatures of orientation and its time dependence are absent. To that end, we discuss the time dependence of the coherent rotational motion associated with electronically resonant one-photon excitations. We illustrate our findings with calculated two-dimensional scattering signals for the sodium fluoride molecule (NaF) in the gas phase.

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Section: Simulations and Discussionmentioning

confidence: 76%

Time-resolved x-ray scattering from impulsively aligned or oriented molecules

2020

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Violation of centrosymmetry in time-resolved ultrafast-electron diffraction from vibrating oriented diatomic molecules

Shao

Starace

2020

Phys. Rev. A

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Probing Electronic Fluxes via Time-Resolved X-Ray Scattering

et al. 2020

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The current flux density is a vector field that can be used to describe theoretically how electrons flow in a system out-of-equilibrium. In this work, we unequivocally demonstrate that the signal obtained from time-resolved X-ray scattering does not only map the time-evolution of the electronic charge distribution, but also encodes information about the associated electronic current flux density. We show how the electronic current flux density qualitatively maps the distribution of electronic momenta and reveals the underlying mechanism of ultrafast charge migration processes, while also providing quantitative information about the timescales of electronic coherences.Time-resolved imaging (TRI) of dynamically evolving electronic charge distribution is essential for complete understanding of complex chemical and biological processes in nature. Moreover, TRI of valence electron charge distribution is paramount to understand different instances during chemical reactions such as conformational changes, charge migration, and bond formation and breakage [1][2][3][4]. Following the quantum mechanical version of continuity equation, the flow of electron charge distribution is accompanied by associated electronic fluxes [5]. The concept of quantum electronic fluxes offers a wealth of crucial informations and has played a decisive role for understanding the mechanism of chemical reactions [6][7][8]. However, the notion of electronic fluxes has been restricted to theoretical modelling [9-18] and there is no general way to probe them directly in experiment. In this work, we will demonstrate a real-space and real-time imaging of electronic fluxes associated with attosecond non-stationary charge migration using time-resolved X-ray scattering (TRXS). For this purpose, we will consider benzene molecule as a test system in which a pump pulse will induce an adiabatic charge migration and ultrashort X-ray pulses will probe the electronic fluxes accompanying charge migration.Scattering of X-rays from matter is an indispensable technique to unveil the real-space structure of solids, biomolecules and molecules with atomic-scale spatial resolution [19]. Tremendous technological progress has been made to generate tunable ultraintense and ultrashort Xray pulses from X-ray free-electron lasers (XFELs) [20][21][22]. X-ray pulses with few femtoseconds pulse duration are routinely generated at various XFELs (LCLS, SACLA, European XFEL). Moreover, few successful attempts have been demonstrated to generate attosecond X-ray pulses [23][24][25][26][27][28]. The availability of these ultrashort X-ray pulses offer to extend X-ray scattering from static to time domain with unprecedented temporal resolution [29,30]. Scattering of ultrashort X-ray pulses from the temporarily evolving electronic charge distribution promises to provide stroboscopic snap-shots of matter in action with atomic-scale spatial and temporal resolutions [31,32]. A direct approach to envision TRXS is a pump-probe experiment, where the pump pulse triggers the ultrafast dynamics ...

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Violation of centrosymmetry in time-resolved coherent x-ray diffraction from rovibrational states of diatomic molecules

Cited by 3 publications

References 73 publications

Time-resolved x-ray scattering from impulsively aligned or oriented molecules

Time-resolved x-ray scattering from impulsively aligned or oriented molecules

Violation of centrosymmetry in time-resolved ultrafast-electron diffraction from vibrating oriented diatomic molecules

Probing Electronic Fluxes via Time-Resolved X-Ray Scattering

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