Radicals in aqueous solution: Assessment of density-corrected SCAN functional


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{
  "id": "1782", 
  "updated": "2023-05-31T09:15:27.984139+00:00", 
  "metadata": {
    "version": 1, 
    "contributors": [
      {
        "givennames": "Fabian", 
        "affiliations": [
          "Department of Chemistry, University of Zurich (UZH), CH-8057 Zurich, Zurich, Switzerland"
        ], 
        "email": "fabian.belleflamme@chem.uzh.ch", 
        "familyname": "Belleflamme"
      }, 
      {
        "givennames": "Juerg", 
        "affiliations": [
          "Department of Chemistry, University of Zurich (UZH), CH-8057 Zurich, Zurich, Switzerland"
        ], 
        "email": "hutter@chem.uzh.ch", 
        "familyname": "Hutter"
      }
    ], 
    "title": "Radicals in aqueous solution: Assessment of density-corrected SCAN functional", 
    "_oai": {
      "id": "oai:materialscloud.org:1782"
    }, 
    "keywords": [
      "Density-corrected DFT", 
      "Density functional theory", 
      "r2SCAN", 
      "Aqueous hydroxyl radical", 
      "Aqueous sulfanyl radical", 
      "Methanethiol", 
      "Hydrogen sulfide"
    ], 
    "publication_date": "May 31, 2023, 11:15:27", 
    "_files": [
      {
        "key": "OHradical.tar.gz", 
        "description": "Hydroxyl radical solvated in 63 water molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.", 
        "checksum": "md5:36dcd11def7cdff7d23ffce7015065a3", 
        "size": 1559375286
      }, 
      {
        "key": "SHradical.tar.gz", 
        "description": "Sulfanyl radical solvated in 63 water molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.", 
        "checksum": "md5:4b6c65972b84b9b99359d28043b86621", 
        "size": 1563532825
      }, 
      {
        "key": "CH3S_CH3SH.tar.gz", 
        "description": "Radical cation cluster [CH\u2083S\u2234CH\u2083SH]\u207a solvated in 64 water molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.", 
        "checksum": "md5:b61b72ec1ac1adc5bc1a667ca498539a", 
        "size": 1601696095
      }, 
      {
        "key": "HS_SH2.tar.gz", 
        "description": "Radical cation cluster [SH\u2234SH\u2082]\u207a solvated in 62 water molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.", 
        "checksum": "md5:025520107d4777e44becfc770a7fbacc", 
        "size": 1516869193
      }, 
      {
        "key": "H2O.tar.gz", 
        "description": "Bulk liquid water of 64 molecules. Provided are input files for CP2K, and 30ps trajectories generated from this input.", 
        "checksum": "md5:1257fc80410f5129854b660c65b54fe2", 
        "size": 1076874768
      }
    ], 
    "references": [
      {
        "comment": "Submitted manuscript where the data is discussed", 
        "citation": "F. Belleflamme, J. Hutter, PCCP, (2023) (submitted)", 
        "type": "Journal reference"
      }
    ], 
    "description": "We study self-interaction effects in solvated and strongly-correlated cationic molecular clusters, with a focus on the solvated hydroxyl radical. To address the self-interaction issue, we apply the DC-r\u00b2SCAN method, with the auxiliary density matrix approach. Validating our method through simulations of bulk liquid water, we demonstrate that DC-r\u00b2SCAN maintains the structural accuracy of r\u00b2SCAN while effectively addressing spin density localization issues. Extending our analysis to solvated cationic molecular clusters, we find that the hemibonded motif in the [CH\u2083S\u2234CH\u2083SH]\u207a cluster is disrupted in the DC-r\u00b2SCAN simulation, in contrast to r\u00b2SCAN that preserves the (three-electron-two-center)-bonded motif. Similarly, for the [SH\u2234SH\u2082]\u207a cluster, r\u00b2SCAN restores the hemibonded motif through spin leakage, while DC-r\u00b2SCAN predicts a weaker hemibond formation influenced by solvent-solute interactions. Our findings demonstrate the potential of DC-r\u00b2SCAN combined with the auxiliary density matrix method to improve electronic structure calculations, providing insights into the properties of solvated cationic molecular clusters. This work contributes to the advancement of self-interaction corrected electronic structure theory and offers a computational framework for modeling condensed phase systems with intricate correlation effects.", 
    "status": "published", 
    "license": "Creative Commons Attribution 4.0 International", 
    "conceptrecid": "1781", 
    "is_last": true, 
    "mcid": "2023.85", 
    "edited_by": 576, 
    "id": "1782", 
    "owner": 768, 
    "license_addendum": null, 
    "doi": "10.24435/materialscloud:y4-7s"
  }, 
  "revision": 5, 
  "created": "2023-05-30T16:22:07.218696+00:00"
}