Converged Colored Noise Path Integral Molecular Dynamics Study of the Zundel Cation Down to Ultralow Temperatures at Coupled Cluster Accuracy

“On-the-fly” coupled cluster-based path-integral molecular dynamics simulations predict that the effective potential of the protonated water–dimer has a single-well only.

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Density Functionals with Quantum Chemical Accuracy: From Machine Learning to Molecular Dynamics

10.26434/chemrxiv.8079917.v1 ◽

2019 ◽

Cited By ~ 4

Author(s):

Mihail Bogojeski ◽

Leslie Vogt-Maranto ◽

Mark E. Tuckerman ◽

Klaus-Robert Mueller ◽

Kieron Burke

Keyword(s):

Machine Learning ◽

Molecular Dynamics ◽

Quantum Chemical ◽

Density Functional ◽

Md Simulations ◽

Training Data ◽

Coupled Cluster ◽

Density Functionals ◽

Cluster Accuracy ◽

Single Water Molecule

<div> <div> <div> <p>Kohn-Sham density functional theory (DFT) is a standard tool in most branches of chemistry, but accuracies for many molecules are limited to 2-3 kcal/mol with presently-available functionals. <i>Ab initio </i>methods, such as coupled-cluster, routinely produce much higher accuracy, but computational costs limit their application to small molecules. We create density functionals from coupled-cluster energies, based only on DFT densities, via machine learning. These functionals attain quantum chemical accuracy (errors below 1 kcal/mol). Moreover, density-based ∆-learning (learning only the correction to a standard DFT calculation, ∆-DFT) significantly reduces the amount of training data required. We demonstrate these concepts for a single water molecule, and then illustrate how to include molecular symmetries with ethanol. Finally, we highlight the robustness of ∆-DFT by correcting DFT simulations of resorcinol on the fly to obtain molecular dynamics (MD) trajectories with coupled-cluster accuracy. Thus ∆-DFT opens the door to running gas-phase MD simulations with quantum chemical accuracy, even for strained geometries and conformer changes where standard DFT is quantitatively incorrect. </p> </div> </div> </div>

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Correction: “On-the-fly” coupled cluster path-integral molecular dynamics: impact of nuclear quantum effects on the protonated water dimer

Physical Chemistry Chemical Physics ◽

10.1039/c5cp90118a ◽

2015 ◽

Vol 17 (29) ◽

pp. 19673-19674 ◽

Cited By ~ 2

Author(s):

Thomas Spura ◽

Hossam Elgabarty ◽

Thomas D. Kühne

Keyword(s):

Molecular Dynamics ◽

Path Integral ◽

Quantum Effects ◽

Chem Phys ◽

Water Dimer ◽

Coupled Cluster ◽

Cluster Path ◽

Nuclear Quantum Effects ◽

Phys Chem Chem Phys

Correction for “On-the-fly” coupled cluster path-integral molecular dynamics: impact of nuclear quantum effects on the protonated water dimer` by Thomas Spura et al., Phys. Chem. Chem. Phys., 2015, 17, 14355–14359.

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Ab initio path integral molecular dynamics simulation study on the dihydrogen bond of NH4+⋯BeH2

Chemical Physics Letters ◽

10.1016/j.cplett.2005.05.035 ◽

2005 ◽

Vol 410 (1-3) ◽

pp. 54-58 ◽

Cited By ~ 12

Author(s):

Aiko Hayashi ◽

Motoyuki Shiga ◽

Masanori Tachikawa

Keyword(s):

Molecular Dynamics ◽

Molecular Dynamics Simulation ◽

Ab Initio ◽

Path Integral ◽

Simulation Study ◽

Dynamics Simulation ◽

Dihydrogen Bond

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Car–Parrinello and path integral molecular dynamics study of the intramolecular hydrogen bonds in the crystals of benzoylacetone and dideuterobenzoylacetone

Physical Chemistry Chemical Physics ◽

10.1039/c4cp02569e ◽

2014 ◽

Vol 16 (42) ◽

pp. 23026-23037 ◽

Cited By ~ 16

Author(s):

Piotr Durlak ◽

Zdzisław Latajka

Keyword(s):

Molecular Dynamics ◽

Hydrogen Bond ◽

Hydrogen Bonds ◽

Ab Initio ◽

Path Integral ◽

Molecular Crystal ◽

Short Hydrogen Bond ◽

Deuterated Analogue ◽

Dynamics Simulations ◽

Intramolecular Hydrogen

The dynamics of the intramolecular short hydrogen bond in the molecular crystal of benzoylacetone and its deuterated analogue are investigated using ab initio molecular dynamics simulations.

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