Related papers: NATPS: Nonadiabatic Transition Path Sampling Using…
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…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
Using a generalized energy-conserving transition probability, it is shown how nonadiabatic calculations, within the Wigner-Heisenberg representation of quantum mechanics, can be reliably extended to far longer times than those allowed by a…
Nonadiabatic couplings (NACs) play a crucial role in modeling photochemical and photophysical processes with methods such as the widely used fewest-switches surface hopping (FSSH). There is therefore a strong incentive to machine learn NACs…
Simulating transition dynamics between metastable states is a fundamental challenge in dynamical systems and stochastic processes with wide real-world applications in understanding protein folding, chemical reactions and neural activities.…
We present a model intended for rapid sampling of ground and excited state potential energy surfaces for first-row transition metal active sites. The method is computationally inexpensive and is suited for dynamics simulations where (1)…
We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…
Many chemical reactions can be formulated in terms of particle diffusion in a complex energy landscape. Transition path theory (TPT) is a theoretical framework for describing the direct (reaction) pathways from reactant to product states…
Recently proposed non-adiabatic ring polymer molecular dynamics (NRPMD) approach has shown to provide accurate quantum dynamics by incorporating explicit electronic state descriptions and nuclear quantizations. Here, we present a rigorous…
Distributed stateful stream processing enables the deployment and execution of large scale continuous computations in the cloud, targeting both low latency and high throughput. One of the most fundamental challenges of this paradigm is…
This article reviews the concepts and methods of variational path sampling. These methods allow computational studies of rare events in systems driven arbitrarily far from equilibrium. Based upon a statistical mechanics of trajectory space…
Exceptional points (EPs) have attracted extensive research interest due to their intriguing properties. One of the hallmarks of EP physics is that dynamically encircling the EPs induces chiral mode switching, arising from the breakdown of…
The mixed quantum-classical dynamical simulation is essential to study nonadiabatic phenomena in photophysics and photochemistry. In recent years, many machine learning models have been developed to accelerate the time evolution of the…
We propose a scheme which can produce desired nonadiabatic passages for the stimulated Raman transition in three-level systems. The state transfer in the protocol is realized by following the evolution of the dynamical basis itself and no…
Adiabatic evolutions find widespread utility in applications to quantum state engineering, geometric quantum computation, and quantum simulation. Although offering robustness to experimental imperfections, adiabatic processes are…
Computer simulations generate trajectories at a single, well-defined thermodynamic state point. Statistical reweighting offers the means to reweight static and dynamical properties to different equilibrium state points by means of analytic…
We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…
The powerful molecular dynamics (MD) simulation is basically based on a picture that the atoms experience classical-like trajectories under the exertion of classical force field determined by the quantum mechanically solved electronic…
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…
Temperature-accelerated sliced sampling (TASS) is a well-established enhanced sampling method that facilitates exhaustive exploration of high-dimensional collective variable (CV) space through directed sampling employing a combination of…