相关论文: Multi-messenger tracking of coherence loss during …
Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…
When a chemical bond is broken, the molecular structure undergoes a transformation. An ideal experiment should probe the change in the electronic and nuclear structure simultaneously. Here, we present a method for the simultaneous…
We first argue that the covalent bond and the various closed-shell interactions can be thought of as symmetry broken versions of one and the same interaction, viz., the multi-center bond. We use specially chosen molecular units to show that…
Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on few- to sub-femtosecond time scales. While recent attosecond experiments have addressed…
The development of attosecond technology has enabled the real-time observation of coherent electron motion in atoms, molecules and condensed phases. Experimentally, it is now possible to generate laser pulses of durations of only a few tens…
Current-induced bond rupture is a fundamental process in nanoelectronic architectures such as molecular junctions and in scanning tunneling microscopy measurements of molecules at surfaces. The understanding of the underlying mechanisms is…
Photoionization using attosecond pulses can lead to the formation of coherent superpositions of the electronic states of the parent ion. However, ultrafast electron ejection triggers not only electronic but also nuclear dynamics---leading…
A coherent superposition of two electronic states of ozone (ground and Hartley B) is prepared with a UV pump pulse. Using the multiconfiguration time-dependent Hartree approach, we calculate the subsequent time evolution of the two…
Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic…
After core-ionization of CO$_2$, typically an Auger-Meitner decay takes place, leading to the formation of a dicationic molecule that may dissociate into CO$^+$ and O$^+$. We demonstrate experimentally that the recoil momentum of the…
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…
The distortion on the intermittency signal, due to detection efficiency and to the presence of pre--equilibrium emitted particles, is studied in a schematic model of nuclear multi- fragmentation. The source of the intermittency signal is…
Using a combination of high-level ab initio electronic structure methods with efficient on-the-fly semiclassical evaluation of nuclear dynamics, we performed a massive scan of small polyatomic molecules searching for a long lasting…
In a double-slit experiment with a bipartite system, the visibility of interference fringes depends on the availability of which-way information. Here, we report the formation of a Bell-like state of photoelectron and residual ion in the…
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…
Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We…
The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the…
We demonstrate the breakdown of molecular-frame dynamics induced by the uncoupling of molecular rotation from electronic motion in molecular Rydberg states. We observe this non-Born-Oppenheimer regime in the time domain through…
Electronic coherences are key to understanding and controlling photo-induced molecular transformations. We identify a crucial quantum-mechanical feature of electron-nuclear correlation, the projected nuclear quantum momenta, essential to…
In time-resolved photoemission experiments, more than one electron can be emitted from the solid by a single ultra-short pulse. We theoretically demonstrate how correlations between the momenta of outgoing electrons relate to time-dependent…