Power Series Approximation for the Correlation Kernel Leading to Kohn-Sham Methods Combining Accuracy, Computational Efficiency, and General Applicability
| Autor: | Jannis Erhard, Andreas Görling, Patrick Bleiziffer |
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| Rok vydání: | 2016 |
| Předmět: |
Power series
010304 chemical physics Computer science General Physics and Astronomy Kohn–Sham equations Multireference configuration interaction Electronic structure Type (model theory) 01 natural sciences Correlation kernel 0103 physical sciences Applied mathematics Gravitational singularity 010306 general physics Scaling |
| Zdroj: | Physical Review Letters. 117 |
| ISSN: | 1079-7114 0031-9007 |
| DOI: | 10.1103/physrevlett.117.143002 |
| Popis: | A power series approximation for the correlation kernel of time-dependent density-functional theory is presented. Using this approximation in the adiabatic-connection fluctuation-dissipation (ACFD) theorem leads to a new family of Kohn-Sham methods. The new methods yield reaction energies and barriers of unprecedented accuracy and enable a treatment of static (strong) correlation with an accuracy of high-level multireference configuration interaction methods but are single-reference methods allowing for a black-box-like handling of static correlation. The new methods exhibit a better scaling of the computational effort with the system size than rivaling wave-function-based electronic structure methods. Moreover, the new methods do not suffer from the problem of singularities in response functions plaguing previous ACFD methods and therefore are applicable to any type of electronic system. |
| Databáze: | OpenAIRE |
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