A dual-cutoff machine-learned potential for condensed organic systems obtained uncertainty-guided active learning.

Machine-learned potentials (MLPs) trained on data combine the computational efficiency of classical interatomic potentials with the accuracy and generality of the first-principles method used in the creation of the respective training set. In this work, we implement and train a MLP to obtain an accurate description of the potential energy surface and property predictions for organic compounds, as both single molecules and in the condensed phase. We devise a dual descriptor, based on the atomic cluster expansion (ACE), that couples an information-rich short-range description with a coarser long-range description that captures weak intermolecular interactions.

Amorphous cis-1,4-polybutadiene P-V-T properties from atomistic simulations.

Context: As a result of the diversity of microstructures encountered in cis-1,4-polybutadiene and the variety of measurement methods used, experimental values of variation of glass transition temperature (Tg) with pressure are relatively dispersed. However, atomistic simulations enable access to valuable information for very well-controlled chemistry and structures with a well-defined and systematic acquisition protocol. By varying the temperature and pressure, the specific volume of the melt was computed, yielding results that deviated by only 2% from experimental data.

Prediction of ionic conductivity from adiabatic heating in non-equilibrium molecular dynamics on various test systems.

Context: The evaluation of ionic conductivity through atomistic modeling typically involves calculating diffusion coefficients, which often necessitates simulations spanning several hundreds of nanoseconds. This study introduces a less computationally demanding approach based on non-equilibrium molecular dynamics applicable to a wide range of systems.

Method: Ionic conductivity is determined by evaluating the Joule heating effect recorded during non-equilibrium molecular dynamics (NEMD) simulations.

Computing thermomechanical properties of dry homopolymers used as raw materials for formulation of biomedical hydrogels.

Different static properties have been calculated with COMPASS force field for polyacrylamide, poly(2-hydroxyethylacrylate) (HEA), poly(2-hydroxyethylmethacrylate) (HEMA), poly(glycidylmethacrylate) (GMA), polyethylene glycol (PEG), and poly(2,2,2-trifluoroethylmethacrylate) (TFEM). For each polymers, the calculated values were averaged on five equilibrated configurations of amorphous cell composed of one atactic chain containing 100 repeat units. The ranking obtained from the densities calculated at 300 K is TFEM > HEA ≈ xpolycrylamide > HEMA ≈ GMA > PEG.

Density functional theory calculations on azobenzene derivatives: a comparative study of functional group effect.

Density functional theory (DFT) calculations have been used to investigate the structural properties, dipole moments, polarizabilities, Gibbs energies, hardness, electronegativity, HOMO/LUMO energies, and chemical potentials of trans and cis configurations of eight para-substituted azobenzene derivatives. All properties have been obtained using the B3LYP functional and 6-31++G(d,p) basis set. The planar structures have been obtained for all optimized trans configurations.

Decomposition mechanisms of trinitroalkyl compounds: a theoretical study from aliphatic to aromatic nitro compounds.

The chemical mechanisms involved in the decomposition of trinitroethyl compounds were studied for both aliphatic and aromatic derivatives using density functional theory calculations. At first, in the case of 1,1,1-trinitrobutane, used as a reference molecule, two primary channels were highlighted among the five investigated ones: the breaking of the C-N bond and the HONO elimination. Then, the influence of various structural parameters was studied for these two reactions by changing the length of the carbon chain, adding substituents or double bonds along the carbon chain.

A DFT study on the initial stage of thermal degradation of Poly(methyl methacrylate)/carbon nanotube system.

DFT calculations, with VWN exchange correlation functional and double numeric basis set, were used to evaluate the energies required for the scission reactions taking place in the initial stage of the thermal degradation of Poly(methyl methacrylate) (PMMA) in the presence of a carbon nanotube (CNT). Side group and main chain scissions were investigated. The results averaged from five configurations of pure PMMA (DP=5) were used as references and compared to the results obtained for the five same configurations of PMMA grafted on three carbon nanotubes of similar diameter (1.

Calculations of the charge distribution in dodecyltrimethylammonium: a quantum chemical investigation.

In this work we report the atomic partial charges evaluated on dodecyltrimethylammonium ion. The values obtained from 17 quantum methods [CHELP, CHELPG, MK, NPA at (HF, LDA, PBE, B3LYP)//6-31G++(d,p) level and APT at B3LYP//6-31G++(d,p)] on the molecule optimised at B3LYP/6-31G++(d,p) level were compared to two semiempirical methods (Gasteiger and Qeq) and the commercial force field PCFF. All methods based on quantum calculation gave a positive charge delocalised on at least the first four alkyl groups of the tail.

Density functional theory characterisation of 4-hydroxyazobenzene.

We report the structural properties, infrared (IR) and Raman spectra, dipole moment, polarisability, hardness and chemical potential of the trans and cis configurations of 4-hydroxyazobenzene calculated using the B3LYP functionals. All calculations were performed with the following basis sets: 6-31G, 6-31++G, 6-31G(d,p), 6-31++G(d,p), 6-31G(2d,2p), 6-31++G(2d,2p) and 6-311++G(2d,2p). We observed that 6-31++G(d,p) gives similar results to 6-311++G(2d,2p).