Replication Data for: Static polarizabilities at the basis set limit: A benchmark of 124 species

DOI

Introduction This Dataverse entry contains replication data for our journal article “Static polarizabilities at the basis set limit: A benchmark of 124 species” published in Journal of Chemical Theory and Computation. It contains highly precise static polarizabilities computed in multiwavelet basis in combination with density functional theory (DFT, PBE functional). In addition, the d/Preliminaryata set contains analysis tools (Jupyter Notebooks with Python3 code) for generating the figures in the journal article.

How to use Because our multiwavelet data is guaranteed to be at the complete basis set limit (to within the specified limit), it is suitable as a benchmark reference in studies of static polarizabilities where the basis set convergence is important. With multiwavelets we don't have to assume that the computed property is at the basis set limit, as is the case with Gaussian type orbital (GTO) basis sets, and it is therefore possible to confirm whether the property of interest computed basis is sufficiently converged with respect to the complete basis set limit. Our benchmark reference can also be used in the development of new methodology that requires accurate training data.

Running the Jupyter Notebooks The Anaconda Python distribution is usually recommended for obtaining Jupyter Notebook. It can be downloaded from here: https://www.anaconda.com/distribution/

The simplest way to run the notebooks is to download all files in this DataverseNO dataset. That will preserve the directory structure, which is absolutely necessary to avoid errors. Then start your Jupyter Notebook session, navigate to the data set directory, and open the desired notebook.

Journal article Brakestad et al. "Static polarizabilities at the basis set limit: A benchmark of 124 species". J. Chem. Theory Comput. (2020)

Abstract from journal article Benchmarking molecular properties with Gaussian-type orbital (GTO) basis sets can be challenging, because one has to assume that the computed property is at the complete basis set (CBS) limit, without a robust measure of the error. Multiwavelet (MW) bases can be systematically improved with a controllable error, which eliminates the need for such assumptions. In this work, we have used MWs within Kohn–Sham density functional theory to compute static polarizabilities for a set of 92 closed-shell and 32 open-shell species. The results are compared to recent benchmark calculations employing the GTO-type aug-pc4 basis set. We observe discrepancies between GTO and MW results for several species, with open-shell systems showing the largest deviations. Based on linear response calculations, we show that these discrepancies originate from artefacts caused by the field strength, and that several polarizabilies from a previous study were contaminated by higher order responses (hyperpolarizabilities). Based on our MW benchmark results, we can affirm that aug-pc4 is able to provide results close to the CBS limit, as long as finite-difference effects can be controlled. However, we suggest that a better approach is to use MWs, which are able to yield precise finite-difference polarizabilities even with small field strengths.

ORCA, 4.1.2

MRChem, 0

Python, 3.6

Identifier
DOI https://doi.org/10.18710/KLQVOK
Related Identifier https://doi.org/10.1021/acs.jctc.0c00128
Metadata Access https://dataverse.no/oai?verb=GetRecord&metadataPrefix=oai_datacite&identifier=doi:10.18710/KLQVOK
Provenance
Creator Brakestad, Anders (UiT The Arctic University of Norway); Jensen, Stig Rune (UiT The Arctic University of Norway); Wind, Peter (UiT The Arctic University of Norway); D'Alessandro, Marco (Istituto di Struttura della Materia); Genovese, Luigi (Laboratoire de Simulation Atomistique); Hopmann, Kathrin Helen (UiT The Arctic University of Norway); Frediani, Luca (UiT The Arctic University of Norway)
Publisher DataverseNO
Contributor Frediani, Luca; UiT The Arctic University of Norway; UiT Open Research Data
Publication Year 2020
Funding Reference Research Council of Norway; Notur - The Norwegian Metacenter for Computational Science
Rights CC0 Waiver
OpenAccess true
Contact Frediani, Luca (UiT The Arctic University of Norway)
Representation
Resource Type benchmark data
Format text/plain; chemical/x-xyz; application/x-ipynb+json; application/octet-stream; text/x-python; text/tab-separated-values
Size 4125; 16320; 53519; 309298; 182295; 11129; 86; 91695; 4442; 1949; 75002; 73951; 84000; 18597; 46380; 7439; 49943; 85403; 162938; 4021; 59752; 71738; 34328; 13119; 1946; 205; 10644
Version 4.1
Discipline Chemistry;Physics
Spatial Coverage Tromsø, Norway