175 research outputs found
Machine Learning for Quantum Mechanical Properties of Atoms in Molecules
We introduce machine learning models of quantum mechanical observables of
atoms in molecules. Instant out-of-sample predictions for proton and carbon
nuclear chemical shifts, atomic core level excitations, and forces on atoms
reach accuracies on par with density functional theory reference. Locality is
exploited within non-linear regression via local atom-centered coordinate
systems. The approach is validated on a diverse set of 9k small organic
molecules. Linear scaling of computational cost in system size is demonstrated
for saturated polymers with up to sub-mesoscale lengths
Variational Transition State Theory-Based Surface Chemistry for the C2H6/H2/O2/Pt System
Application of computational chemistry methods to obtain thermodynamic data for hydrogen production from liquefied petroleum gas
Benchmark thermochemistry of the C_nH_{2n+2} alkane isomers (n=2--8) and performance of DFT and composite ab initio methods for dispersion-driven isomeric equilibria
The thermochemistry of linear and branched alkanes with up to eight carbons
has been reexamined by means of W4, W3.2lite and W1h theories. `Quasi-W4'
atomization energies have been obtained via isodesmic and hypohomodesmotic
reactions. Our best atomization energies at 0 K (in kcal/mol) are: 1220.04
n-butane, 1497.01 n-pentane, 1774.15 n-hexane, 2051.17 n-heptane, 2328.30
n-octane, 1221.73 isobutane, 1498.27 isopentane, 1501.01 neopentane, 1775.22
isohexane, 1774.61 3-methylpentane, 1775.67 diisopropyl, 1777.27 neohexane,
2052.43 isoheptane, 2054.41 neoheptane, 2330.67 isooctane, and 2330.81
hexamethylethane. Our best estimates for are: -30.00
n-butane, -34.84 n-pentane, -39.84 n-hexane, -44.74 n-heptane, -49.71 n-octane,
-32.01 isobutane, -36.49 isopentane, -39.69 neopentane, -41.42 isohexane,
-40.72 3-methylpentane, -42.08 diisopropyl, -43.77 neohexane, -46.43
isoheptane, -48.84 neoheptane, -53.29 isooctane, and -53.68 hexamethylethane.
These are in excellent agreement (typically better than 1 kJ/mol) with the
experimental heats of formation at 298 K obtained from the CCCBDB and/or NIST
Chemistry WebBook databases. However, at 0 K a large discrepancy between theory
and experiment (1.1 kcal/mol) is observed for only neopentane. This deviation
is mainly due to the erroneous heat content function for neopentane used in
calculating the 0 K CCCBDB value. The thermochemistry of these systems,
especially of the larger alkanes, is an extremely difficult test for density
functional methods. A posteriori corrections for dispersion are essential.
Particularly for the atomization energies, the B2GP-PLYP and B2K-PLYP
double-hybrids, and the PW6B95 hybrid-meta GGA clearly outperform other DFT
functionals.Comment: (J. Phys. Chem. A, in press
Estimating reaction constants by ab initio molecular modeling: a study on the oxidation of phenol to catechol and hydroquinone in advanced oxidation processes
The proton affinity of proline analogs using the kinetic method with full entropy analysis
Application of the Correlation Consistent Composite Approach (ccCA) to Third-Row (Ga-Kr) Molecules
Cyclic Versus Linear Isomers Produced by Reaction of the Methylidyne Radical (CH) with Small Unsaturated Hydrocarbons
Design, synthesis, fabrication and simulation of conjugated molecule for detection of lithium ions
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