Abstract
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.
- Received 24 March 2016
DOI:https://doi.org/10.1103/PhysRevLett.117.143002
© 2016 American Physical Society
Physics Subject Headings (PhySH)
Viewpoint
Improving Electronic Structure Calculations
Published 26 September 2016
A new approach to calculating the properties of molecules and solids may offer higher accuracy at reasonable computational cost, accelerating the discovery of useful materials.
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