{"@context":{"@vocab":"https://cir.nii.ac.jp/schema/1.0/","rdfs":"http://www.w3.org/2000/01/rdf-schema#","dc":"http://purl.org/dc/elements/1.1/","dcterms":"http://purl.org/dc/terms/","foaf":"http://xmlns.com/foaf/0.1/","prism":"http://prismstandard.org/namespaces/basic/2.0/","cinii":"http://ci.nii.ac.jp/ns/1.0/","datacite":"https://schema.datacite.org/meta/kernel-4/","ndl":"http://ndl.go.jp/dcndl/terms/","jpcoar":"https://github.com/JPCOAR/schema/blob/master/2.0/"},"@id":"https://cir.nii.ac.jp/crid/1363670320596203264.json","@type":"Article","productIdentifier":[{"identifier":{"@type":"DOI","@value":"10.1063/1.1834563"}},{"identifier":{"@type":"URI","@value":"https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/1.1834563/10873521/044103_1_online.pdf"}}],"dc:title":[{"@value":"Improving the orbital-free density functional theory description of covalent materials"}],"description":[{"type":"abstract","notation":[{"@value":"<jats:p>The essential challenge in orbital-free density functional theory (OF-DFT) is to construct accurate kinetic energy density functionals (KEDFs) with general applicability (i.e., transferability). During the last decade, several linear-response (LR)-based KEDFs have been proposed. Among them, the Wang-Govind-Carter (WGC) KEDF, containing a density-dependent response kernel, is one of the most accurate that still affords a linear scaling algorithm. For nearly-free-electron-like metals such as Al and its alloys, OF-DFT employing the WGC KEDF produces bulk properties in good agreement with orbital-based Kohn-Sham (KS) DFT predictions. However, when OF-DFT, using the WGC KEDF combined with a recently proposed bulk-derived local pseudopotential (BLPS), was applied to semiconducting and metallic phases of Si, problems arose with convergence of the self-consistent density and energy, leading to poor results. Here we provide evidence that the convergence problem is very likely caused by the use of a truncated Taylor series expansion of the WGC response kernel. Moreover, we show that a defect in the ansatz for the first-order reduced density matrix underlying the LR KEDFs limits the accuracy of these KEDFs. By optimizing the two free parameters involved in the WGC KEDF, the two-body Fermi wave vector mixing parameter γ and the reference density ρ* used in the Taylor expansion, OF-DFT calculations with the BLPS can achieve semiquantitative results for nine phases of bulk silicon. These new parameters are recommended whenever the WGC KEDF is used to study nonmetallic systems.</jats:p>"}]}],"creator":[{"@id":"https://cir.nii.ac.jp/crid/1383670320596203265","@type":"Researcher","foaf:name":[{"@value":"Vincent L. Ligneres"}],"jpcoar:affiliationName":[{"@value":"Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095-1569"},{"@value":"Department of Chemistry, Princeton University, Princeton, New Jersey 08544"}]},{"@id":"https://cir.nii.ac.jp/crid/1383670320596203392","@type":"Researcher","foaf:name":[{"@value":"Emily A. Carter"}],"jpcoar:affiliationName":[{"@value":"Department of Chemistry and Biochemistry, University of California, Los Angele, Los Angeles, California 90095-1569"},{"@value":"Department of Mechanical and Aerospace Engineering and Program in Applied and Computational Mathematics, Princeton University, Princeton, New Jersey 08544"}]},{"@id":"https://cir.nii.ac.jp/crid/1383670320596203264","@type":"Researcher","foaf:name":[{"@value":"Baojing Zhou"}],"jpcoar:affiliationName":[{"@value":"Department of Chemistry and Biochemistry, University of California, Los Angeles, Los Angeles, California 90095-1569"}]}],"publication":{"publicationIdentifier":[{"@type":"PISSN","@value":"00219606"},{"@type":"EISSN","@value":"10897690"}],"prism:publicationName":[{"@value":"The Journal of Chemical Physics"}],"dc:publisher":[{"@value":"AIP Publishing"}],"prism:publicationDate":"2005-01-04","prism:volume":"122","prism:number":"4","prism:startingPage":"044103"},"reviewed":"false","url":[{"@id":"https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/1.1834563/10873521/044103_1_online.pdf"}],"createdAt":"2005-01-15","modifiedAt":"2023-07-09","relatedProduct":[{"@id":"https://cir.nii.ac.jp/crid/1360004233922730880","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["isReferencedBy"],"jpcoar:relatedTitle":[{"@value":"Semi-local machine-learned kinetic energy density functional with third-order gradients of electron density"}]},{"@id":"https://cir.nii.ac.jp/crid/1360005516777713024","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["isReferencedBy"],"jpcoar:relatedTitle":[{"@value":"Orbital-free density functional theory calculation applying semi-local machine-learned kinetic energy density functional and kinetic potential"}]},{"@id":"https://cir.nii.ac.jp/crid/1360294643711454208","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["isReferencedBy"],"jpcoar:relatedTitle":[{"@value":"Order-\n<mml:math xmlns:mml=\"http://www.w3.org/1998/Math/MathML\"><mml:mi>N</mml:mi></mml:math>\n orbital-free density-functional calculations with machine learning of functional derivatives for semiconductors and metals"}]},{"@id":"https://cir.nii.ac.jp/crid/1361412891661211648","@type":"Article","resourceType":"学術雑誌論文(journal article)","relationType":["isReferencedBy"],"jpcoar:relatedTitle":[{"@value":"Semi-local machine-learned kinetic energy density functional demonstrating smooth potential energy curves"}]}],"dataSourceIdentifier":[{"@type":"CROSSREF","@value":"10.1063/1.1834563"},{"@type":"CROSSREF","@value":"10.1063/1.5007230_references_DOI_W0AYrL6Ax4D9Lz0jm0r3ZmxguVp"},{"@type":"CROSSREF","@value":"10.1103/physrevresearch.3.033198_references_DOI_W0AYrL6Ax4D9Lz0jm0r3ZmxguVp"},{"@type":"CROSSREF","@value":"10.1016/j.cplett.2020.137358_references_DOI_W0AYrL6Ax4D9Lz0jm0r3ZmxguVp"},{"@type":"CROSSREF","@value":"10.1016/j.cplett.2019.136732_references_DOI_W0AYrL6Ax4D9Lz0jm0r3ZmxguVp"}]}