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A variational formulation of the Harris functional as correction to linear-scaling subsystem density functional theory

Fabian Belleflamme1*, Anna-Sophia Hehn1, Marcella Iannuzzi1, Juerg Hutter1

1 Department of Chemistry, University of Zurich (UZH), CH-8057 Zurich, Zurich, Switzerland

* Corresponding authors emails: fabian.belleflamme@chem.uzh.ch
DOI10.24435/materialscloud:fq-y7 [version v1]

Publication date: Aug 31, 2022

How to cite this record

Fabian Belleflamme, Anna-Sophia Hehn, Marcella Iannuzzi, Juerg Hutter, A variational formulation of the Harris functional as correction to linear-scaling subsystem density functional theory, Materials Cloud Archive 2022.109 (2022), doi: 10.24435/materialscloud:fq-y7.

Description

Accurate descriptions of intermolecular interactions are of great importance in simulations of molecular liquids. We present a novel method that combines in a variational formulation the accuracy of the Harris functional approach with the computational efficiency of linear-scaling subsystem density functional theory (DFT). While subsystem DFT methods allow for efficient large-scale simulations, they often lack in accuracy. The proposed method allows for simulations with millihartree accuracy in comparison to the Kohn-Sham DFT reference, at near linear-scaling efficiency. Embedded in the CP2K program package, the method is designed to enable ab initio molecular dynamics simulations of molecular solutions for system sizes of several thousands of atoms. As example of production applications we applied the method to molecular dynamics simulations in the isobaric-isothermal ensemble of the binary mixtures cyclohexane-methanol and toluene-methanol at different molar fractions of methanol. This record contains all CP2K input files necessary for the MD simulations, as well as 30ps trajectory files.

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Files

File name Size Description
TOL100.tar.gz
MD5md5:b90fb65340694e4ccc6e169be45aac52
1.9 GiB Liquid of 100 toluene molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
TOL80.tar.gz
MD5md5:54b69ef63f8b9ecefd660368627c4329
1.6 GiB Binary liquid mixture of 80 toluene and 20 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
TOL60.tar.gz
MD5md5:aad35aa449b4e3c5233cfdc2ef4674c1
1.4 GiB Binary liquid mixture of 60 toluene and 40 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
TOL40.tar.gz
MD5md5:2ce9d2fcf0c9d2c58ae72889de43436c
1.2 GiB Binary liquid mixture of 40 toluene and 60 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
TOL20.tar.gz
MD5md5:aed584c7322ebabbe15ce1b0327ace02
981.4 MiB Binary liquid mixture of 20 toluene and 80 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
CHX100.tar.gz
MD5md5:c2e3c9f654b8b9f7610615f6e64f8426
2.2 GiB Liquid of 100 cyclohexane molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
CHX80.tar.gz
MD5md5:bf68b8feda409513e3fd33c28538640a
1.9 GiB Binary liquid mixture of 80 cyclohexane and 20 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input
CHX60.tar.gz
MD5md5:2fbb435f80158f9008cfd643be029440
1.6 GiB Binary liquid mixture of 60 cyclohexane and 40 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input
CHX40.tar.gz
MD5md5:e0696a27f1817c713e776580be621bda
1.3 GiB Binary liquid mixture of 40 cyclohexane and 60 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input
CHX20.tar.gz
MD5md5:685e92d831946ac9022e1649d7fa58d6
1.0 GiB Binary liquid mixture of 20 cyclohexane and 80 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input
MOH500.tar.gz
MD5md5:161fa4ec2a65316133a39f35a2d9c215
3.7 GiB Liquid of 500 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.
MOH100.tar.gz
MD5md5:947a7f4518aeda5ea48d0ad2b9bc12e1
755.4 MiB Liquid of 100 methanol molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Preprint (Preprint where the data is discussed)
F. Belleflamme, A. Hehn, M. Iannuzzi, J. Hutter, A Variational Formulation of the Harris Functional as Correction to Linear-Scaling Subsystem Density Functional Theory, submitted to The Journal of Chemical Physics)

Keywords

SNSF Harris functional Subsystem DFT Linear-scaling DFT molecular dynamics simulation Cyclohexane Toluene Methanol CP2K isobaric-isothermal ensemble

Version history:

2022.109 (version v1) [This version] Aug 31, 2022 DOI10.24435/materialscloud:fq-y7