Related papers: Investigating Photoinduced Proton Coupled Electron…
We apply a recently developed quasi-diabatic (QD) scheme to the symmetric quasi-classical (SQC) approach for accurate quantum dynamics propagation. By using the adiabatic states as the quasi-diabatic states during a short-time quantum…
We develop a detailed theoretical model of photo-induced proton-coupled electron transfer (PPCET) processes, which are at the basis of solar energy harvesting in biological systems and photovoltaic materials. Our model enables to analyze…
This paper provides the first ab-initio on-the-fly example of using the Quasi-Diabatic (QD) scheme for non-adiabatic simulations with diabatic dynamics approaches. The QD scheme provides a seamless interface between diabatic quantum…
We introduce a simple method for characterizing reactive pathways in quantum systems. Flux auto- correlation and cross-correlation functions are employed to develop a quantitative measure of dynamical coupling in quantum transition events,…
We generalize the quasi-diabatic (QD) propagation scheme to simulate the non-adiabatic polariton dynamics in molecule-cavity hybrid systems. The adiabatic-Fock states, which are the tensor product states of the adiabatic electronic states…
Electron transfer is an important and fundamental process in chemistry, biology and physics, and has received significant attention in recent years. Perhaps one of the most intriguing questions concerns with the realization of the…
Excited state proton transfer is an ubiquitous phenomenon in biology and chemistry, spanning from the ultrafast reactions of photo-bases and acids to light-driven, enzymatic catalysis and photosynthesis. However, the simulation of such…
Here we report an observation of cation-dependent nonadiabaticity in a proton-coupled electron transfer electrode process (PCET) during hydrogen evolution at electrified interfaces of Au(111) single-crystal electrode and electrolytes by…
We present a real-time path integral theory for the rate of electron transfer reactions. Using graph theoretic techniques, the dynamics is expressed in a formally exact way as a set of integral equations. With a simple approximation for the…
Proton-coupled electron transfer (PCET) is foundational to catalysis, bioenergetics, and energy conversion, yet capturing and disentangling the coupled motions of electrons, protons, and solvent has remained a major experimental challenge.…
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…
Proton-coupled electron transfers (PCET) are elementary steps in electrocatalysis. However, accurate calculations of PCET rates remain challenging, especially considering nuclear quantum effects (NQEs) under a constant potential condition.…
We perform on-the-fly non-adiabatic molecular dynamics simulations using the symmetrical quasi-classical (SQC) approach with the recently suggested molecular Tully models: ethylene and fulvene. We attempt to provide benchmarks of the SQC…
A novel method of coherent manipulation of the electron tunneling in quantum-dots is proposed, which utilizes the quantum interference in nonadiabatic double-crossing of the discrete energy levels. In this method, we need only a smoothly…
The coupled quantum dynamics of electrons and protons is ubiquitous in many dynamical processes involving light-matter interaction, such as solar energy conversion in chemical systems and photosynthesis. A first-principles description of…
We present a detailed derivation and numerical tests of a new mixed quantum-classical scheme to deal with non-adiabatic processes. The method is presented as the zero-th order approximation to the exact coupled dynamics of electrons and…
Proton-coupled electron transfer (PCET) is the underlying mechanism governing important reactions ranging from water splitting in photosynthesis to oxygen reduction in hydrogen fuel cells. The interplay of proton and electronic charge…
We review recent theoretical calculations of charge transfer through mesoscopic devices in response to slowly-oscillating, spatially-confined, potentials. The discussion is restricted to non-interacting electrons, and emphasizes the role of…
Periodically driven systems have emerged as a useful technique to engineer the properties of quantum systems, and are in the process of being developed into a standard toolbox for quantum simulation. An outstanding challenge that leaves…
We review a scheme for the systematic design of quantum control protocols based on shortcuts to adiabaticity in few-level quantum systems. The adiabatic dynamics is accelerated by introducing high-frequency modulations in the control…