相关论文: First-Principles Approach for Coupled Quantum Dyna…
Photocatalysis induced by sunlight is one of the most promising approach to environmental protection, solar energy conversion and sustainable production of fuels. The computational modeling of photocatalysis is a rapidly expending field…
A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…
Plasmonic nanocavities are a promising platform for strong light-matter coupling and enhanced spectroscopies at the single-molecule level. These nanoscale environments are challenging to model due to their strongly multimodal character and…
We present an application of our new theoretical formulation of quantum dynamics, moment propagation theory (MPT) (Boyer et al., J. Chem. Phys. 160, 064113 (2024)), for employing machine-learning techniques to simulate the quantum dynamics…
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…
The combined quantum electron-nuclear dynamics is often associated with the Born-Huang expansion of the molecular wave function and the appearance of nonadiabatic effects as a perturbation. On the other hand, native multicomponent…
Nuclear quantum effects and non-Born--Oppenheimer effects play a vital role in many chemical and biological processes, motivating the incorporation of such effects into dynamical simulations. In real-time nuclear--electronic orbital…
Within the nuclear-electronic orbital (NEO) framework, the real-time NEO time-dependent density functional theory (RT-NEO-TDDFT) approach enables the simulation of coupled electronic-nuclear dynamics. In this approach, the electrons and…
The theoretical description of materials' properties driven out of equilibrium has important consequences in various fields such as semiconductor spintronics, nonlinear optics, continuous and discrete quantum information science and…
In density functional-theoretic studies of photoionized water-based systems, the role of charge localization in proton-transfer dynamics is not well understood. This is due to the inherent complexity in extracting the contributions of…
The experimental observation of collective behaviour in proton-proton and proton-nucleus collisions poses a fundamental theoretical question regarding the proper characterization of the initial state underlying hydrodynamic evolution. While…
Proton transfer is central to many processes of chemical interest. The simulation of proton transfer dynamics requires the inclusion of nuclear quantum effects, such as zero-point energy, nuclear delocalization, and tunneling. Herein, we…
In ion irradiation processes, electronic stopping power describes the energy transfer rate from the irradiating ion to the target material's electrons. Due to the scarcity and significant uncertainties in experimental electronic stopping…
We present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear-electronic orbital (NEO) theory and real-time time-dependent density functional theory (RT-TDDFT) for extended periodic systems. In addition to a quantum…
Ab initio techniques have revolutionised the way in which theory can help practitioners to explore critical mechanisms that govern reactions or properties, and to develop new strategies for materials discovery and design. Yet, their…
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…
We study the dynamics of initial nucleation processes of photoinduced structural change of molecular crystals. In order to describe the nonadiabatic transition in each molecule, we employ a model of localized electrons coupled with a fully…
Hydrogen bonding interactions between biological chromophores and their surrounding protein and solvent environment significantly affect the photochemical pathways of the chromophore and its biological function. A common first step in the…
A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…
Quantum proton tunneling (QPT) in the two representative multi-electron/-proton transfer electrode processes, i.e. hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR), was investigated by using polycrystalline platinum…