Imaging interatomic electron current in crystals with ultrafast resonant x-ray scattering

Popova-Gorelova, Daria; Santra, Robin

doi:10.1103/physrevb.92.184304

Cited by 19 publications

(31 citation statements)

References 52 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Therefore, angle-resolved photoelectron spectra do not follow the time evolution of the electron density. A similar effect that a measured signal from an electronic wave packet does not follow the time-dependent electron density has been shown for time-resolved resonant [23,24] and nonresonant [21] x-ray scattering patterns as well as time-resolved electron diffraction patterns [40].…”

Section: Figmentioning

confidence: 72%

“…Alternatively to ultrafast resonant x-ray scattering [23,24], one can use time-and angle-resolved photoelectron spectroscopy to obtain real-space information on instantaneous charge distributions and electron currents in molecules. Recent progress in attosecond science makes an experimental implementation of this technique feasible in the near future [14].…”

Section: Discussionmentioning

confidence: 99%

“…In these studies, the effect of the broad bandwidth of an ultrashort probe pulse has either been neglected [17,18,20] or approximated [19]. However, we have earlier demonstrated that an accurate treatment within the quantum electrodynamics (QED) approach taking into account all transitions that can be induced by a broadband probe pulse is necessary for a correct description of ultrafast x-ray scattering from a nonstationary electronic system [21][22][23][24]. Therefore, since this should also be true for time-resolved photoelectron imaging, we apply the QED treatment to describe the interaction of a nonstationary electronic system with an ultrashort isolated probe pulse inducing single-photon ionization.…”

Section: Introductionmentioning

confidence: 99%

“…We describe the interaction between the electronic system and the photoionizing ultrashort probe pulse using a similar formalism to the one applied for the study of ultrafast x-ray scattering [21][22][23][24]. Since we assume that the probe pulse does not temporally overlap with the pump pulse, the interaction of the electronic system with the probe pulse can be considered independently from the pump pulse [25].…”

mentioning

confidence: 99%

See 3 more Smart Citations

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

2016

Self Cite

View full text Add to dashboard Cite

We theoretically study how time-and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time-and angle-resolved photoelectron spectra. We show how a Fourier analysis of time-and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.

show abstract

Section: Figmentioning

confidence: 72%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

mentioning

confidence: 99%

See 2 more Smart Citations

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

2016

Self Cite

View full text Add to dashboard Cite

show abstract

“…Depending on the symmetry of the orbitals, one obtains different dynamics (e.g., wiggling or breathing modes), which can then be probed by the scattering scheme at hand. There are some works, on resonant x-ray scattering, that deal with more complex systems, such as Br 2 , (KBr) 108 , and (Ge) 83 [71,72]. In all earlier works on attosecond x-ray scattering, the preparation of the initial states was not considered explicitly.…”

Section: Dynamics Of Armentioning

confidence: 99%

Attosecond x-ray scattering from a particle-hole wave packet

2017

View full text Add to dashboard Cite

We investigate the imaging of electron wave-packet dynamics by measuring the pattern of inelastically scattered photons. For this purpose, we develop a theory of time-resolved Compton scattering. We demonstrate that, by using a sufficiently short x-ray pulse, the scattering cross section directly reflects the instantaneous momentum density of the electron. Therefore, we propose time-resolved Compton scattering as a tool to image electron wave-packet dynamics in momentum space. To illustrate this, we simulate electron wave packets in argon by using the time-dependent configuration-interaction singles method. Specifically, we consider coherent particle-hole wave packets, where the hole is in either the 3p or the 3s shell, and the particle (the excited electron) is either in a Rydberg state or in the continuum. Our calculations confirm that the dynamics of electron wave packets can indeed be imaged by measuring the doubly differential Compton scattering cross section. When the x-ray detector has no energy resolution at all, the contribution of Compton scattering to the differential scattering cross section becomes stationary. In that case, the motion of the particle and the hole can no longer be inferred from the scattering pattern.

show abstract

Probing Electronic Symmetry Reduction during Charge Migration via Time‐Resolved X‐Ray Diffraction

et al. 2022

View full text Add to dashboard Cite

The present work focuses on probing ultrafast charge migration after symmetry-breaking excitation using ultrashort laser pulses. LiCN is chosen as prototypical system because it can be oriented in the laboratory frame and it possesses opticallyaccessible charge transfer states at low energies. The charge migration is simulated within the hybrid time-dependent density functional theory/configuration interaction framework. Time-resolved electronic current densities and simulated timeresolved x-ray diffraction signals are used to unravel the mechanism of charge migration. Our simulations demonstrate that specific choices of laser polarization lead to a control over the symmetry of the induced charge migration. Moreover, timeresolved x-ray diffraction signals are shown to encode transient symmetry reduction at intermediate times.

show abstract

Imaging interatomic electron current in crystals with ultrafast resonant x-ray scattering

Cited by 19 publications

References 52 publications

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

Attosecond x-ray scattering from a particle-hole wave packet

Probing Electronic Symmetry Reduction during Charge Migration via Time‐Resolved X‐Ray Diffraction

Contact Info

Product

Resources

About