The ground states of Lennard-Jones clusters for sizes up to n=147 are estimated as a function of the de Boer quantum delocalization length Lambda , and the n-Lambda "phase diagram" is constructed. The increase in Lambda favors more disordered and diffuse structures over more symmetric and compact ones, eventually making the liquidlike motif most energetically favorable. The analogy between the quantum- and thermally-induced structural transitions is explored.
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http://dx.doi.org/10.1103/PhysRevE.79.022101 | DOI Listing |
J Phys Chem Lett
January 2025
University of Maryland Computer-Aided Drug Design Center, Department of Pharmaceutical Sciences, School of Pharmacy, University of Maryland, Baltimore, Maryland 21201, United States.
An improvement in the computational efficiency of polarizable force field simulations is made through the development of a polarizable Drude water model, SWM3, in combination with the use of Lennard-Jones Particle Mesh Ewald (LJPME) for the treatment of long-range LJ interactions. The experimental bulk properties, density, heat of vaporization, dielectric constant, and self-diffusion constant of the SWM3 model are accurately replicated at ambient condition. The temperature dependence of the bulk properties is also captured except for the density.
View Article and Find Full Text PDFJ Chem Theory Comput
November 2024
University of Maryland Computer-Aided Drug Design Center, Department of Pharmaceutical Sciences, School of Pharmacy, University of Maryland, Baltimore, Maryland 21201, United States.
In this work the 4-point polarizable SWM4 Drude water model is reparametrized. Multiple models were developed using different strategies toward reproduction of specific target data. Results indicate that no individual model can reproduce all the selected target data in the context of the present form of the potential energy function.
View Article and Find Full Text PDFSoft Matter
December 2024
Biomacromolecular Systems and Processes, Institute of Biological Information Processing, Forschungszentrum Jülich, 52428 Jülich, Germany.
Competing short-range attractive (SA) and long range repulsive (LR) particle interactions can be used to describe three-dimensional charge-stabilized colloid or protein dispersions at low added salt concentrations, as well as membrane proteins with interaction contributions mediated by lipid molecules. Using Langevin dynamics (LD) simulations, we determine the generalized phase diagram, cluster shapes and size distributions of a generic quasi-two-dimensional (Q2D) dispersion of spherical SALR particles confined to in-plane motion inside a bulk fluid. The SA and LR interaction parts are modelled by a generalized Lennard-Jones potential and a screened Coulomb potential, respectively.
View Article and Find Full Text PDFACS Omega
October 2024
Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53705, United States.
The conversion of lignin can produce biomass-derived aromatic compounds such as 2-pyrone-4,6-dicarboxylic acid (PDC), which is a potential sustainable precursor of bioplastics. PDC is a pseudoaromatic dicarboxylic acid that can aggregate in aqueous solution. Aggregation depends upon PDC-PDC, PDC-water, and PDC-ion interactions that are representative of interactions in similar charged, aromatic compounds.
View Article and Find Full Text PDFJ Chem Phys
September 2024
Department of Chemical and Biomedical Engineering, Cleveland State University, Cleveland, Ohio 44115, USA.
A novel statistical mechanical methodology is applied to clusters of N ≤ 7 atoms. Exact statistical analogs for any energy derivative of entropy ∂mS/∂Em are used in rigorous microcanonical Monte Carlo simulations to vastly enlarge the pool of measurable thermodynamic properties relative to previous work. All analogs are given for two alternative partition functions of the microcanonical ensemble.
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