Discontinuous Nature of the Exchange-Correlation Functional in Strongly Correlated Systems
Standard approximations for the exchange-correlation functional have been found to give big errors for the linearity condition of fractional charges, leading to delocalization error, and the constancy condition of fractional spins, leading to static correlation error. These two conditions are now un...
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| Vydané v: | Physical review letters Ročník 102; číslo 6; s. 066403 |
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| Hlavní autori: | , , |
| Médium: | Journal Article |
| Jazyk: | English |
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United States
13.02.2009
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| ISSN: | 0031-9007, 1079-7114 |
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| Abstract | Standard approximations for the exchange-correlation functional have been found to give big errors for the linearity condition of fractional charges, leading to delocalization error, and the constancy condition of fractional spins, leading to static correlation error. These two conditions are now unified and extended to states with both fractional charge and fractional spin to give a much more stringent condition: the exact energy functional is a plane, linear along the fractional charge coordinate and constant along the fractional spin coordinate with a line of discontinuity at the integer. Violation of this condition underlies the failure of all known approximate functionals to describe the gaps in strongly correlated systems. It is shown that explicitly discontinuous functionals of the density or orbitals that go beyond these currently used smooth approximations is the key for the application of density functional theory to strongly correlated systems. |
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| AbstractList | Standard approximations for the exchange-correlation functional have been found to give big errors for the linearity condition of fractional charges, leading to delocalization error, and the constancy condition of fractional spins, leading to static correlation error. These two conditions are now unified and extended to states with both fractional charge and fractional spin to give a much more stringent condition: the exact energy functional is a plane, linear along the fractional charge coordinate and constant along the fractional spin coordinate with a line of discontinuity at the integer. Violation of this condition underlies the failure of all known approximate functionals to describe the gaps in strongly correlated systems. It is shown that explicitly discontinuous functionals of the density or orbitals that go beyond these currently used smooth approximations is the key for the application of density functional theory to strongly correlated systems.Standard approximations for the exchange-correlation functional have been found to give big errors for the linearity condition of fractional charges, leading to delocalization error, and the constancy condition of fractional spins, leading to static correlation error. These two conditions are now unified and extended to states with both fractional charge and fractional spin to give a much more stringent condition: the exact energy functional is a plane, linear along the fractional charge coordinate and constant along the fractional spin coordinate with a line of discontinuity at the integer. Violation of this condition underlies the failure of all known approximate functionals to describe the gaps in strongly correlated systems. It is shown that explicitly discontinuous functionals of the density or orbitals that go beyond these currently used smooth approximations is the key for the application of density functional theory to strongly correlated systems. Standard approximations for the exchange-correlation functional have been found to give big errors for the linearity condition of fractional charges, leading to delocalization error, and the constancy condition of fractional spins, leading to static correlation error. These two conditions are now unified and extended to states with both fractional charge and fractional spin to give a much more stringent condition: the exact energy functional is a plane, linear along the fractional charge coordinate and constant along the fractional spin coordinate with a line of discontinuity at the integer. Violation of this condition underlies the failure of all known approximate functionals to describe the gaps in strongly correlated systems. It is shown that explicitly discontinuous functionals of the density or orbitals that go beyond these currently used smooth approximations is the key for the application of density functional theory to strongly correlated systems. |
| ArticleNumber | 066403 |
| Author | Mori-Sánchez, Paula Yang, Weitao Cohen, Aron J. |
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| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/19257614$$D View this record in MEDLINE/PubMed |
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| Cites_doi | 10.1103/PhysRevB.77.115123 10.1126/science.1158722 10.1063/1.1712502 10.1103/PhysRevA.26.1200 10.1103/PhysRevA.76.040501 10.1063/1.1589733 10.1103/PhysRevLett.84.5172 10.1103/PhysRevB.78.201103 10.1103/PhysRevB.44.943 10.1103/PhysRevLett.49.1691 10.1103/PhysRevLett.100.146401 10.1002/qua.560240302 10.1063/1.2741248 10.1103/PhysRevLett.79.2089 10.1209/epl/i2002-00261-y 10.1063/1.2987202 10.1103/PhysRev.140.A1133 10.1103/PhysRevLett.51.1888 10.1103/PhysRevLett.51.1884 |
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| References | PhysRevLett.102.066403Cc5R1 PhysRevLett.102.066403Cc16R1 PhysRevLett.102.066403Cc6R1 PhysRevLett.102.066403Cc17R1 PhysRevLett.102.066403Cc3R1 PhysRevLett.102.066403Cc14R1 PhysRevLett.102.066403Cc4R1 PhysRevLett.102.066403Cc15R1 PhysRevLett.102.066403Cc1R1 PhysRevLett.102.066403Cc2R1 PhysRevLett.102.066403Cc18R1 PhysRevLett.102.066403Cc19R1 PhysRevLett.102.066403Cc20R1 PhysRevLett.102.066403Cc10R1 J. P. Perdew (PhysRevLett.102.066403Cc13R1) 1986; 19 PhysRevLett.102.066403Cc21R1 PhysRevLett.102.066403Cc11R1 PhysRevLett.102.066403Cc9R1 PhysRevLett.102.066403Cc7R1 PhysRevLett.102.066403Cc8R1 |
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