相关论文: Modeling solid-liquid interface reactions with nex…
We present a framework for atomistic simulations of surface catalysis under electrochemical bias. The framework makes use of extended Lagrangian Born-Oppenheimer quantum-based molecular dynamics (XL-BOMD) simulations, which provide the…
Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) [Phys. Rev. Lett. vol. 100, 123004 (2008)] is combined with Kohn-Sham density functional theory (DFT) using a DFT+U correction based on the Hubbard model. This combined…
A shadow molecular dynamics scheme for flexible charge models is presented, where the shadow Born-Oppenheimer potential is derived from a coarse-grained approximation of range-separated density functional theory. The interatomic potential,…
Extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) in its most recent shadow potential energy version has been implemented in the semiempirical PyTorch-based software PySeQM. The implementation includes finite electronic…
Extended Lagrangian Born-Oppenheimer molecular dynamics [Phys. Rev. Lett., ${\bf 100}$, 123004 (2008)] is formulated for general Hohenberg-Kohn density functional theory and compared to the extended Lagrangian framework of first principles…
An alternative method is introduced to solve a simple two-dimensional models describing vibrational excitation and dissociation processes during the electron-molecule collisions. The model works with one electronic and one nuclear degree of…
Extended Lagrangian Born-Oppenheimer molecular dynamics [{\em Phys.\ Rev.\ Lett.\ } {\bf 2008}, {\em 100}, 123004] is presented for Hartree-Fock theory, where the extended electronic degrees of freedom are represented by a density matrix,…
Extended Lagrangian molecular dynamics (XLMD) is a general method for performing molecular dynamics simulations using quantum and classical many-body potentials. Recently several new XLMD schemes have been proposed and tested on several…
Understanding the evolution of electrified solid-liquid interfaces during electrochemical reactions is crucial. However, capturing the dynamic behavior of the interfaces with high temporal resolution and accuracy over long timescales…
We present an extension of the shadow extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) method to excited state molecular dynamics (ESMD) in the context of \DeltaSCF Kohn-Sham density functional theory, with demonstrations…
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…
Massively-parallel molecular dynamics simulation is applied to systems containing electrolytes, vapour-liquid interfaces, and biomolecules in contact with water-oil interfaces. Novel molecular models of alkali halide salts are presented and…
Extended Lagrangian Born-Oppenheimer molecular dynamics based on Kohn-Sham density functional theory is generalized in the limit of vanishing self-consistent field optimization prior to the force evaluations. The equations of motion are…
We discuss the development and implementation of a constant temperature (NVT) molecular dynamics scheme that combines the Nos\'e-Hoover chain thermostat with the extended Lagrangian Born-Oppenheimer molecular dynamics (BOMD) scheme, using a…
Graph-based linear scaling electronic structure theory for quantum-mechanical molecular dynamics simulations is adapted to the most recent shadow potential formulations of extended Lagrangian Born-Oppenheimer molecular dynamics, including…
The interfaces between metal electrodes and liquid electrolytes are prototypical in electrochemistry. That is why it is crucial to have a molecular and dynamical understating of such interfaces for both electrical properties and chemical…
While Born-Oppenheimer molecular dynamics (BOMD) has been widely studied by resorting to powerful methods in mathematical analysis, this paper presents a geometric formulation in terms of Hamilton's variational principle and…
We review recent ab initio molecular dynamics studies of electrode/electrolyte interfaces in lithium ion batteries. Our goals are to introduce experimentalists to simulation techniques applicable to models which are arguably most faithful…
Computational studies of electrochemical interfaces based on density-functional theory (DFT) play an increasingly important role in present research on electrochemical processes for energy conversion and storage. The homogeneous background…
In recent years, rapid progress has been made in solid-state lithium batteries. Among various technologies, coating the surface of electrodes or electrolytes has proven to be an effective method to enhance interfacial stability and improve…