A kinetic theory for quantum many-particle systems in time-dependent electromagnetic fields is developed based on a gauge-invariant formulation. The resulting kinetic equation generalizes previous results to quantum systems and includes many-body effects. It is, in particular, applicable to the interaction of strong laser fields with dense correlated plasmas.
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http://dx.doi.org/10.1103/physreve.60.4725 | DOI Listing |
J Chem Theory Comput
January 2025
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States.
We present an implementation of the quantum mechanics/molecular mechanics (QM/MM) method for periodic systems using GPU accelerated QM methods, a distributed multipole formulation of the electrostatics, and a pseudobond treatment of the QM/MM boundary. We demonstrate that our method has well-controlled errors, stable self-consistent QM convergence, and energy-conserving dynamics. We further describe an application to the catalytic kinetics of chorismate mutase.
View Article and Find Full Text PDFChemphyschem
January 2025
University of Namur, Department of Chemistry, Rue de Bruxelles, 61, 5000, Namur, BELGIUM.
The [4+2] Diels-Alder cycloaddition reaction between 2,5-DMF (1) and ethylene derivatives (2a-h) activated by electron-withdrawing groups has been studied at the density functional theory levels using a panoply of tools to unravel the reaction mechanisms. From the analysis of the reactivity indices, 2a-h behave as electrophiles while 1 as nucleophile, and the activation of the double bond of ethylene increases its electrophilicity, which is accompanied by an enhancement of the polarity of the reaction. The activation Gibbs free energy decreases linearly as a function of this increase of polarity, as estimated by the electrophilicity difference between the reactants.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Advanced Computing, Mathematics and Data Division, Pacific Northwest National Laboratory, 902 Battelle Boulevard, P.O. Box 999, MS J7-10, Richland, Washington 99352, USA.
We report the values of the collision integrals, needed for the calculation of the macroscopic transport properties such as viscosity (η) and diffusion coefficient (D) of gases within the Chapman-Enskog kinetic gas theory, for a generalized Lennard-Jones potential (gLJ), a more general potential with an adjustable long range 1/r dependence that can describe a wide range of intermolecular interactions.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Theoretical and Computational Physics Section, Raja Ramanna Centre for Advanced Technology, Indore 452013, India.
The orbital-free density functional theory (OF-DFT) based method is a convenient tool to carry out electronic structure calculations scaling almost linearly with the number of electrons. However, the main impediment in the application of this method is the unavailability of the accurate form for the non-interacting kinetic energy functional in terms of electron density. The Pauli kinetic energy functional is the unknown part of the kinetic energy functional, and the corresponding Pauli potential appears in the governing Euler equation.
View Article and Find Full Text PDFSmall
January 2025
College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, P. R. China.
Nickel hydroxide (Ni(OH)) is considered to be one of the most promising electrocatalysts for urea oxidation reaction (UOR) under alkaline conditions due to its flexible structure, wide composition and abundant 3D electrons. However, its slow electrochemical reaction rate, high affinity for the reaction intermediate *COOH, easy exposure to low exponential crystal faces and limited metal active sites that seriously hinder the further improvement of UOR activities. Herein it is reported electrocatalyst composed of rich oxygen-vacancy (O) defects with amorphous SeO-covered Ni(OH) (O-SeO/Ni(OH)).
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