Exploring energy landscapes of charge multipoles using constrained density functional theory


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{
  "id": "1903", 
  "updated": "2023-09-15T09:24:27.453808+00:00", 
  "metadata": {
    "version": 1, 
    "contributors": [
      {
        "givennames": "Luca", 
        "affiliations": [
          "Materials Theory, ETH Z\u00fcrich, 8093 Z\u00fcrich, Switzerland"
        ], 
        "familyname": "Schaufelberger"
      }, 
      {
        "givennames": "Maximilian E.", 
        "affiliations": [
          "Materials Theory, ETH Z\u00fcrich, 8093 Z\u00fcrich, Switzerland"
        ], 
        "email": "maximilian.merkel@mat.ethz.ch", 
        "familyname": "Merkel"
      }, 
      {
        "givennames": "Aria", 
        "affiliations": [
          "Materials Theory, ETH Z\u00fcrich, 8093 Z\u00fcrich, Switzerland"
        ], 
        "familyname": "Mansouri Tehrani"
      }, 
      {
        "givennames": "Nicola A.", 
        "affiliations": [
          "Materials Theory, ETH Z\u00fcrich, 8093 Z\u00fcrich, Switzerland"
        ], 
        "familyname": "Spaldin"
      }, 
      {
        "givennames": "Claude", 
        "affiliations": [
          "Materials Theory, ETH Z\u00fcrich, 8093 Z\u00fcrich, Switzerland"
        ], 
        "email": "claude.ederer@mat.ethz.ch", 
        "familyname": "Ederer"
      }
    ], 
    "title": "Exploring energy landscapes of charge multipoles using constrained density functional theory", 
    "_oai": {
      "id": "oai:materialscloud.org:1903"
    }, 
    "keywords": [
      "multipoles", 
      "constrained DFT", 
      "perovskite", 
      "electronic instability", 
      "ERC"
    ], 
    "publication_date": "Sep 15, 2023, 11:24:27", 
    "_files": [
      {
        "key": "README.md", 
        "description": "Description of the contents of data.tar.gz and short instructions to rerun the jupyter notebooks and DFT calculations", 
        "checksum": "md5:31320d8114059ab721a390e110269222", 
        "size": 2243
      }, 
      {
        "key": "data.tar.gz", 
        "description": "tar.gz archive with all data and scripts needed to reproduce Figs. 3-7 in the paper", 
        "checksum": "md5:1802d05872649356cd7da729fabcf764", 
        "size": 174924052
      }
    ], 
    "references": [
      {
        "comment": "Paper where the data and plots are discussed", 
        "doi": "10.1103/PhysRevResearch.5.033172", 
        "citation": "L. Schaufelberger, M. E. Merkel, A. M. Tehrani, N. A. Spaldin, C. Ederer, Phys. Rev. Res. 5, 033172 (2023)", 
        "url": "https://link.aps.org/doi/10.1103/PhysRevResearch.5.033172", 
        "type": "Journal reference"
      }, 
      {
        "comment": "Preprint to the paper where the data and plots are discussed", 
        "doi": "10.48550/arXiv.2305.13988", 
        "citation": "L. Schaufelberger, M. E. Merkel, A. M. Tehrani, N. A. Spaldin, C. Ederer, arxiv 2305.13988 (2023)", 
        "url": "https://arxiv.org/abs/2305.13988", 
        "type": "Preprint"
      }
    ], 
    "description": "We present a method to constrain local charge multipoles within density-functional theory. Such multipoles quantify the anisotropy of the local charge distribution around atomic sites and can indicate potential hidden orders. Our method allows selective control of specific multipoles, facilitating a quantitative exploration of the energetic landscape outside of local minima. Thus, it enables a clear distinction between electronically and structurally driven instabilities. We demonstrate the effectiveness of this method by applying it to charge quadrupoles in the prototypical orbitally ordered material KCuF\u2083. We quantify intersite multipole-multipole interactions as well as the energy-lowering related to the formation of an isolated local quadrupole. We also map out the energy as a function of the size of the local quadrupole moment around its local minimum, enabling quantification of multipole fluctuations around their equilibrium value. Finally, we study charge quadrupoles in the solid solution KCu\u2081\u208b\u2093Zn\u2093F\u2083 to characterize the behavior across the tetragonal-to-cubic transition. Our method provides a powerful tool for studying symmetry breaking in materials with coupled electronic and structural instabilities and potentially hidden orders.", 
    "status": "published", 
    "license": "Creative Commons Attribution 4.0 International", 
    "conceptrecid": "1902", 
    "is_last": true, 
    "mcid": "2023.141", 
    "edited_by": 578, 
    "id": "1903", 
    "owner": 566, 
    "license_addendum": null, 
    "doi": "10.24435/materialscloud:sn-kd"
  }, 
  "revision": 5, 
  "created": "2023-09-14T14:55:26.300882+00:00"
}