相关论文: Coherent electronic-vibrational dynamics in deuter…
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…
Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely…
A coherent vibrational wavepacket is launched and manipulated in the symmetric stretch (a$_1$) mode of CBr$_4$, by impulsive stimulated Raman scattering from non-resonant 400 nm laser pump pulses with various peak intensities on the order…
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…
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…
In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond…
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…
We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the…
High harmonic light sources make it possible to access attosecond time-scales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics,…
Quantum coherence is highly involved in photochemical functioning of complex molecular systems. Co-existence and intermixing of electronic and/or vibrational coherences, while never unambiguously identified experimentally, has been proposed…
Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections (CIs), which generate coherences between electronic…
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…
Attosecond transient absorption spectroscopy (ATAS) is becoming an indispensable and powerful tool in the emerging field of attochemistry, while the interpretation of measurements often requires full considerations of the coupling among…
How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…
The basic properties of atoms, molecules and solids are governed by electron dynamics which take place on extremely short time scales. To measure and control these dynamics therefore requires ultrafast sources of radiation combined with…
We report on the observation, characterization, and control of the electron dynamics in ionized argon atoms. We utilized an intense mid-infrared (MIR) pulse to create a coherent superposition of the spin-orbit split ground state of the ion.…
Quantum beats in nonlinear spectroscopy of molecular aggregates are often attributed to electronic phenomena of excitonic systems, while nuclear degrees of freedom are commonly included into models as overdamped oscillations of bath…
We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode.…
Short-in-time, broad-in-energy attosecond or few-femtosecond pulses can excite coherent superpositions of several electronic states in molecules. This results in ultrafast charge oscillations known as charge migration. A key open question…
Due to the electron correlation, a fast removal of an electron from a molecule may create a coherent superposition of cationic states and in this way initiate pure electronic dynamics in which the hole-charge left by ionization migrates…