Related papers: Making peace with random phases: Ab initio conical…
The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat…
We introduce multistate metadynamics for automatic exploration of conical intersection seams between adiabatic Born-Oppenheimer potential energy surfaces in molecular systems. By choosing the energy gap between the electronic states as a…
Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…
At present, several models for quantum computation have been proposed. Adiabatic quantum computation scheme particularly offers this possibility and is based on a slow enough time evolution of the system, where no transitions take place. In…
Many recent experimental ultrafast spectroscopy studies have hinted at non-adiabatic dynamics indicating the existence of conical intersections, but their direct observation remains a challenge. The rapid change of the energy gap between…
Conical intersections (CIs) are seen as the main mediators of nonadiabatic transitions; yet, mixed quantum-classical (MQC) simulations rarely, if ever, sample geometries with exactly degenerate electronic energies. Here we show that this…
We study the ultrafast dynamic process in photoexcited systems and find that the Franck-Condon or Landau-Zener tunneling between the photoexcited state and the ground state is abruptly blocked with increasing the state coupling from…
Adiabatic circuits are heavily investigated since they allow for computations with an asymptotically close to zero energy dissipation per operation - serving as an alternative technology for many scenarios where energy efficiency is…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
We demonstrate coherent control of motional dynamics in trapped Rydberg ions engineered to exhibit a conical intersection between adiabatic potential-energy surfaces. Using quantum optimal control, an optimally shaped electric field drives…
The anomalous dynamical evolution and the crossing of nonadiabatic energy levels are investigated for exactly solvable time-dependent quantum systems through a reverse-engineering scheme. By exploiting a typical driven model, we elucidate…
One of the intriguing effects due to conical intersections is the geometric phase, manifested as destructive quantum interference in the nuclear probability distribution. However, whether such geometric phaseinduced interference can survive…
Nonadiabatic molecular dynamics simulations aim to describe the coupled electron-nuclear dynamics of molecules in excited electronic states. These simulations have been applied to understand a plethora of photochemical and photophysical…
Non-adiabatic dynamics and conical intersections play a central role in the chemistry of most polyatomic molecules, ranging from isomerization to heterocyclic ring opening and avoided photo-damage of DNA. Studying the underpinning…
Dissociative chemisorption is a key process in hydrogen-metal surface chemistry, where nonadiabatic effects due to low-lying electron-hole-pair excitations may affect reaction outcomes. Molecular dynamics with electronic friction…
A dynamical rearrangement in the electronic structure of a molecule can be driven by different phenomena, including nuclear motion, electronic coherence or electron correlation. Recording such electronic dynamics and identifying their fate…
Geometric phases, which accompany the evolution of a quantum system and depend only on its trajectory in state space, are commonly studied in two-level systems. Here, however, we study the adiabatic geometric phase in a weakly anharmonic…
We present a means of studying rare reactive pathways in open quantum systems using Transition Path Theory and ensembles of quantum jump trajectories. This approach allows for elucidation of reactive paths for dissipative, nonadiabatic…
We present a comprehensive computational framework for simulating nonadiabatic molecular dynamics with explicit inclusion of geometric phase (GP) effects. Our approach is based on a generalized two-level Hamiltonian model that can represent…
We present an approach for carrying out non-adiabatic molecular dynamics simulations of systems in which non-adiabatic transitions arise from the coupling between the classical atomic motions and a quasi-continuum of electronic quantum…