Related papers: Non-Adiabatic Electronic and Vibrational Ring-Open…
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…
Conical intersections are ubiquitous in polyatomic molecules and responsible for a wide range of phenomena in chemistry and physics. We introduce and implement a local diabatic representation for the correlated electron-nuclear dynamics…
The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures and reaction mechanism of these many-body quantum objects are defined on the level of…
Nonadiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy…
Linear off-resonant X-ray Raman techniques are capable of detecting the ultrafast electronic coherences generated when a photoexcited wave packet passes through a conical intersection. A hybrid femtosecond or attosecond probe pulse is…
Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We…
Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale…
We study effects of nonadiabatic couplings in a model of a diatomic molecule in the context of attosecond transient absorption spectroscopy. By using a model system consisting of four diabatic electronic states and with a variable strength…
Conical intersections between electronic potential energy surfaces are paradigmatic for the study of non-adiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond…
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…
Nonadiabatic dynamics around an avoid crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules. The present work shows that the topological phase in conical intersection makes the…
The electron motion in atoms and molecules is at the heart of all phenomena in nature that occur outside the nucleus. Recently, ultrafast electron and X-ray imaging tools have been developed to image the ultrafast dynamics of matter in real…
Nonadiabatic ring-polymer molecular dynamics employs the mapping approach to describe nonadiabatic effects within the ring-polymer ansatz. In this paper, it is generalized to allow for the nuclear and electronic degrees of freedom to be…
Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, spectral congestion and spatial delocalization of valence electron wave functions set fundamental limits…
Conical intersections constitute the conceptual bedrock of our working understanding of ultrafast, nonadiabatic processes within photochemistry (and photophysics). Accurate calculation of potential energy surfaces within the vicinity of…
Ab initio modeling of conical intersection dynamics is crucial for various photochemical, photophysical, and biological processes. However, adiabatic electronic states obtained from electronic structure computations involve random phases,…
We propose an imaging technique to follow core-hole wave-packet oscillations in the nitrogen molecule. In this scheme, an attosecond x-ray pulse core-ionizes the nitrogen molecule and a subsequent attosecond x-ray pulse probes the evolution…
In the field of chemistry, where nuclear motion has traditionally been a focal point, we now explore the ultra-rapid electronic motion spanning attoseconds to femtoseconds, demonstrating that it is equally integral and relevant to the…
Photoinduced isomerization reactions, including ring-opening reactions, lie at the heart of many processes in nature. The mechanisms of such reactions are determined by a delicate interplay of coupled electronic and nuclear dynamics…
Ultrafast optical techniques allow to study ultrafast molecular dynamics involving both nuclear and electronic motion.To support interpretation, theoretical approaches are needed that can describe both the nuclear and electron…