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Attosecond photoelectron interferometry based on the combination of an attosecond pulse train and a synchronized infrared field is a fundamental technique for the temporal characterization of attosecond waveforms and for the investigation…
We apply attosecond transient absorption spectroscopy (ATAS) to explore the effects of a nonzero permanent dipole on electron dynamics at the subfemtosecond scale, exemplified in the polar LiF molecule. In contrast with nonpolar systems, a…
On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…
Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and…
A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees…
In molecular systems containing conical intersections (CIs), a nontrivial geometric phase (GP) appears in the nuclear and electronic wave-functions in the adiabatic representation. We study GP effects in nuclear dynamics of an N-dimensional…
Understanding the reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…
Characterizing and localizing electronic energy degeneracies is important for describ-ing and controlling electronic energy flow in molecules. We show, using topological phase considerations that the Renner effect in polyatomic molecules…
In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this…
The vibrational dynamics of adsorbate molecules in single-molecule junctions depend critically on the geometric structure and electronic interactions between molecule and substrate. Vibrations, excited mechanochemically or by external…
We develop a unified quantum geometric framework to understand reactive quantum dynamics. The critical roles of the quantum geometry of adiabatic electronic states in both adiabatic and non-adiabatic quantum dynamics are unveiled. A…
Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…
Solids exposed to intense electric fields release electrons through tunnelling. This fundamental quantum process lies at the heart of various applications, ranging from high brightness electron sources in DC operation to petahertz vacuum…
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…
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…
Conical intersections (CI) between molecular potential energy surfaces with non-vanishing non-adiabatic couplings generally occur in any molecule consisting of at least three atoms. They play a fundamental role in describing the molecular…
We study the generation of electronic ring currents in the presence of nonadiabatic coupling using circularly polarized light. For this, we introduce a solvable model consisting of an electron and a nucleus rotating around a common center…
A nonadiabatic scheme for the description of the coupled electron and nuclear motions in the ozone molecule was proposed recently. An initial coherent nonstationary state was prepared as a superposition of the ground state and the excited…
Conical intersections (CIs) have been widely studied using spectroscopic techniques. However, CIs have mainly been identified by rapid internal conversion transitions that take place after the photoexcitation. Such identifications cannot…
We find that energy surfaces of more than two atoms or molecules interacting via dipole-dipole po- tentials generically possess conical intersections (CIs). Typically only few atoms participate strongly in such an intersection. For the…