相关论文: Energetics and Kinetics of Primary Charge Separati…
We present a detailed analysis of the mechanism of the primary charge separation process in bacterial photosynthesis using real-time path integrals. Direct computer simulations as well as an approximate analytical theory have been employed…
The energy conversion of oxygenic photosynthesis is triggered by primary charge separation in proteins at the photosystem II reaction center. Here, we investigate the impacts of the protein environment and intramolecular vibrations on…
We consider the dependence of the electron transfer in photosynthetic complexes on correlation properties of random fluctuations of the protein environment. The electron subsystem is modeled by a finite network of connected electron…
In purple bacteria, the fundamental charge-separation step that drives the conversion of radiation energy into chemical energy proceeds along one branch - the A branch - of a heterodimeric pigment-protein complex, the reaction center. Here,…
The photosystem II reaction center (PSII-RC) performs the primary energy conversion steps of oxygenic photosynthesis. While the PSII-RC has been studied extensively, the similar timescales of energy transfer and charge separation, and the…
Photoinduced charge-transfer excitations are key to understand the primary processes of natural photosynthesis and for designing photovoltaic and photocatalytic devices. In this paper, we use Bacteriochlorophyll dimers extracted from the…
Photosynthesis transfers energy efficiently through a series of antenna complexes to the reaction center where charge separation occurs. Energy transfer in vivo is primarily monitored by measuring fluorescence signals from the small…
Molecular dynamics simulations are used to study the mechanism and kinetics of hydrated electron diffusion. The electron center of mass is found to exhibit Brownian-type behavior with a diffusion coefficient considerably greater than that…
We report the results of Molecular Dynamics simulations of electron transfer activation parameters of plastocyanin metalloprotein involved as electron carrier in natural photosynthesis. We have discovered that slow, non-ergodic…
Classical molecular dynamics simulations have recently become a standard tool for the study of electrochemical systems. State-of-the-art approaches represent the electrodes as perfect conductors, modelling their responses to the charge…
A general approach to calculate the diabatic surfaces for electron-transfer reactions is presented, based on first-principles molecular dynamics of the active centers and their surrounding medium. The excitation energy corresponding to the…
We present a plane-wave basis set implementation of charge constrained density functional molecular dynamics (CDFT-MD) for simulation of electron transfer reactions in condensed phase systems. Following earlier work of Wu et al. Phys. Rev.…
Photons emitted from high-energy electron beam interactions with high-field systems, such as the upcoming FACET-II experiments at SLAC National Accelerator Laboratory, may provide deep insight into the electron beam's underlying dynamics at…
This study considers electronic transitions within donor-acceptor complexes dissolved in media with macroscopic polarization. The change of the polarizability of the donor-acceptor complex in the course of electronic transition couples to…
Accounting for geometry-induced changes in the electronic distribution in molecular simulation is important for capturing effects such as charge flow, charge anisotropy and polarization. Multipolar force fields have demonstrated their…
Fully polarizable QM/MM approach based on fluctuating charges and fluctuating dipoles, named QM/FQF{\mu} (J. Chem. Theory Comput. 2019, 15 2233-2245), is extended to the calculation of vertical excitation energies of solvated molecular…
Distributed point charge models (DCM) and their minimal variants (MDCM) have been integrated with tools widely used for condensed-phase simulations, including a virial-based barostat and a slow-growth algorithm for thermodynamic…
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 new mechanism for the primary photoinduced charge separation in photosynthesis is proposed. It involves as real intermediate between the excited special pair state P* and the primary charge separated state P+HL- a trip-trip-singlet PTBLT,…
Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the…