Excited-state forces with the Gaussian and augmented plane wave method for the Tamm–Dancoff approximation of time-dependent density functional theory

JSON Export

{
  "updated": "2024-09-23T11:44:39.068959+00:00", 
  "metadata": {
    "_oai": {
      "id": "oai:materialscloud.org:2344"
    }, 
    "version": 1, 
    "is_last": true, 
    "_files": [
      {
        "size": 7425530, 
        "checksum": "md5:2c71d3438bc431ac7018554372b0bd1c", 
        "key": "DATA_FOR_MATERIALS_CLOUD.zip", 
        "description": "Provided are input and corresponding output files for CP2K computations."
      }
    ], 
    "keywords": [
      "Augmented plane wave methods", 
      "Time-dependent density functional theory", 
      "Gaussian basis sets"
    ], 
    "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\u2013Dancoff 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/\u00c5. 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\u2013Bethe\u2013Salpeter 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.", 
    "contributors": [
      {
        "affiliations": [
          "Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich, Switzerland."
        ], 
        "givennames": "Beliz", 
        "email": "beliz.sertcan@chem.uzh.ch", 
        "familyname": "Sertcan G\u00f6kmen"
      }, 
      {
        "affiliations": [
          "Department of Chemistry, University of Zurich, Winterthurerstrasse 190, 8057 Zurich, Switzerland."
        ], 
        "givennames": "J\u00fcrg", 
        "email": "hutter@chem.uzh.ch", 
        "familyname": "Hutter"
      }, 
      {
        "affiliations": [
          "Institute for Physical Chemistry, Christian-Albrechts-University, Max-Eyth-Strasse 1, 24118 Kiel, Germany"
        ], 
        "givennames": "Anna-Sophia", 
        "email": "hehn@pctc.uni-kiel.de", 
        "familyname": "Hehn"
      }
    ], 
    "edited_by": 98, 
    "owner": 1493, 
    "doi": "10.24435/materialscloud:92-b6", 
    "title": "Excited-state forces with the Gaussian and augmented plane wave method for the Tamm\u2013Dancoff approximation of time-dependent density functional theory", 
    "license": "Creative Commons Attribution 4.0 International", 
    "mcid": "2024.140", 
    "id": "2344", 
    "conceptrecid": "2343", 
    "status": "published", 
    "publication_date": "Sep 23, 2024, 13:44:39", 
    "license_addendum": null, 
    "references": [
      {
        "comment": "Corresponding journal reference discussing the method and results referring to the here archived data.", 
        "type": "Journal reference", 
        "url": "https://doi.org/10.1021/acs.jctc.4c00614", 
        "doi": "10.1021/acs.jctc.4c00614", 
        "citation": "B. Sertcan G\u00f6kmen, J. Hutter, A.-S. Hehn, J. Chem. Theory Comput. XXXX, XXX-XXX (2024)."
      }
    ]
  }, 
  "id": "2344", 
  "revision": 4, 
  "created": "2024-09-20T07:51:42.490795+00:00"
}