Beliz Sertcan Gökmen^1*, Jürg Hutter^1*, Anna-Sophia Hehn^2*

1 Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich, Switzerland.

2 Institute for Physical Chemistry, Christian-Albrechts-University, Max-Eyth-Strasse 1, 24118 Kiel, Germany

* Corresponding authors emails: beliz.sertcan@chem.uzh.ch, hutter@chem.uzh.ch, hehn@pctc.uni-kiel.de

DOI10.24435/materialscloud:92-b6 [version v1]

Publication date: Sep 23, 2024

How to cite this record

Beliz Sertcan Gökmen, Jürg Hutter, Anna-Sophia Hehn, Excited-state forces with the Gaussian and augmented plane wave method for the Tamm–Dancoff approximation of time-dependent density functional theory, Materials Cloud Archive 2024.140 (2024), https://doi.org/10.24435/materialscloud:92-b6

Description

Augmented plane wave methods enable an efficient description of atom-centered or localized features of the electronic density, circumventing high energy cutoffs and thus prohibitive computational costs of pure plane wave formulations. To complement existing implementations for ground-state properties and excitation energies, we present the extension of the Gaussian and augmented plane wave method to excited-state nuclear gradients within the Tamm–Dancoff approximation of time-dependent density functional theory and its implementation in the CP2K program package. Benchmarks for a test set of 35 small molecules demonstrate that maximum errors in the nuclear forces for excited states of singlet and triplet spin multiplicity are smaller than 0.1 eV/Å. The method is furthermore applied to the calculation of the zero-phonon line of defective hexagonal boron nitride. This spectral feature is reproduced with an error of 0.6 eV in comparison to GW–Bethe–Salpeter reference computations and 0.4 eV in comparison to experimental measurements. Accuracy assessments and applications thus demonstrate the potential use of the outlined developments for large-scale applications on excited-state properties of extended systems. The data in this record are supplementary data to the published article with DOI 10.1021/acs.jctc.4c00614.

Materials Cloud sections using this data

Files

File name	Size	Description
DATA_FOR_MATERIALS_CLOUD.zip MD5md5:2c71d3438bc431ac7018554372b0bd1c	7.1 MiB	Provided are input and corresponding output files for CP2K computations.

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External references

Keywords

Augmented plane wave methods Time-dependent density functional theory Gaussian basis sets