Journal ArticleDOI
Molecular model for aqueous ferrous–ferric electron transfer
TLDR
In this article, a molecular model for studying the prototypical ferric-ferrous electron transfer process in liquid water is presented, and the validity of the tight binding model is examined.Abstract:
We present a molecular model for studying the prototypical ferric–ferrous electron transfer process in liquid water, and we discuss its structural implications. Treatment of the nonequilibrium dynamics will be the subject of future work. The elementary constituents in the model are classical water molecules, classical ferric ions (i.e., Fe3+ particles), and a quantal electron. Pair potentials and pseudopotentials describing the interactions between these constituents are presented. These interactions lead to ligand structures of the ferric and ferrous ions that are in good agreement with those observed in nature. The validity of the tight binding model is examined. With umbrella sampling, we have computed the diabatic free energy of activation for electron transfer. The number obtained, roughly 20 kcal/mol, is in reasonable accord with the aqueous ferric–ferrous transfer activation energy of about 15 to 20 kcal/mol estimated from experiment. The Marcus relation for intersecting parabolic diabatic free ene...read more
Citations
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Journal ArticleDOI
Proton-Coupled Electron Transfer
David R. Weinberg,Christopher J. Gagliardi,Jonathan F. Hull,Christine Fecenko Murphy,Caleb A. Kent,Brittany C. Westlake,Amit Paul,Daniel H. Ess,Dewey G. McCafferty,Thomas J. Meyer +9 more
TL;DR: Proton-coupled electron transfer is an important mechanism for charge transfer in a wide variety of systems including biology- and materials-oriented venues and several are reviewed.
Journal ArticleDOI
Contemporary Issues in Electron Transfer Research
TL;DR: In this paper, a qualitative discussion of electron transfer, its time and distance scales, energy curves, and basic parabolic energy models are introduced to define the electron transfer process, and some of the important, challenging, and problematic issues in contemporary electron transfer research are discussed.
Journal ArticleDOI
Simulation of enzyme reactions using valence bond force fields and other hybrid quantum/classical approaches
Johan Åqvist,Arieh Warshel +1 more
TL;DR: Simulation of Enzyme Reactions Using Valence Bond Force Fields and Other Hybrid Quantum/Classical Approaches as mentioned in this paper is an example of a hybrid approach that combines classical and quantum approaches.
Journal ArticleDOI
The dynamics of solvation in polar liquids
TL;DR: In this paper, a review of recent experiments, theories, and computer simulations aimed at elucidating the dynamics of solvation in polar liquids are critically reviewed, and the results of these experiments are presented.
Journal ArticleDOI
Ring-Polymer Molecular Dynamics: Quantum Effects in Chemical Dynamics from Classical Trajectories in an Extended Phase Space
TL;DR: This model, which involves classical evolution in an extended ring-polymer phase space, provides a practical approach to approximating the effects of quantum fluctuations on the dynamics of condensed-phase systems.
References
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Book
CRC Handbook of Chemistry and Physics
TL;DR: CRC handbook of chemistry and physics, CRC Handbook of Chemistry and Physics, CRC handbook as discussed by the authors, CRC Handbook for Chemistry and Physiology, CRC Handbook for Physics,
Journal ArticleDOI
Optimization by Simulated Annealing
TL;DR: There is a deep and useful connection between statistical mechanics and multivariate or combinatorial optimization (finding the minimum of a given function depending on many parameters), and a detailed analogy with annealing in solids provides a framework for optimization of very large and complex systems.
Journal ArticleDOI
A unified formulation of the constant temperature molecular dynamics methods
TL;DR: In this article, the authors compared the canonical distribution in both momentum and coordinate space with three recently proposed constant temperature molecular dynamics methods by: (i) Nose (Mol. Phys., to be published); (ii) Hoover et al. [Phys. Rev. Lett. 77, 63 (1983); and (iii) Haile and Gupta [J. Chem. Phys. 79, 3067 (1983).
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Electron transfers in chemistry and biology
Rudolph A. Marcus,Norman Sutin +1 more
TL;DR: In this paper, the electron transfer reactions between ions and molecules in solution have been the subject of considerable experimental study during the past three decades, including charge transfer, photoelectric emission spectra, chemiluminescent electron transfer, and electron transfer through frozen media.
Journal ArticleDOI
Efficient estimation of free energy differences from Monte Carlo data
TL;DR: Near-optimal strategies are developed for estimating the free energy difference between two canonical ensembles, given a Metropolis-type Monte Carlo program for sampling each one, and their efficiency is never less or greater than that obtained by sampling only one ensemble.