TY - JOUR

T1 - A dual-level approach to four-component relativistic density-functional theory

AU - Mizukami, Wataru

AU - Nakajima, Takahito

AU - Hirao, Kimihiko

AU - Yanai, Takeshi

N1 - Funding Information:
This research was supported in part by the Technology Program, ‘High Performance Computing for Multi-Scale and Multi-Physics Phenomena’ of the Japan Science and Technology Agency (JST), and Grant-in-Aid for Scientific Research (B) 19350007, (C) 21550027, and Young Scientists (B) 21750028 from Ministry of Education, Culture, Sports, Science and Technology-Japan (MEXT). We acknowledge Research Center for Computational Science, Okazaki, and are grateful to Dr. Takeshi Sato and Prof. Trond Saue for fruitful discussions.

PY - 2011/5/18

Y1 - 2011/5/18

N2 - An efficient approach to the fully relativistic density-functional theory (DFT) is proposed to accelerate Dirac-Kohn-Sham calculation that uses high-quality basis sets and hybrid exchange-correlation functional. The dual-level approach proposed by Nakajima and Hirao underlies the present method, estimating high-level four-component DFT energy perturbatively from reference density matrix, which is determined by a relatively inexpensive self-consistent calculation using low-quality basis sets and low-cost functional. A further approximation based on Infinite-Order Two-Component relativistic Hamiltonian is incorporated into the low-level treatment. Accuracy and efficiency were examined by benchmark calculation of spectroscopic values for MH, M2 (M = Cu, Ag, and Au), and AtH.

AB - An efficient approach to the fully relativistic density-functional theory (DFT) is proposed to accelerate Dirac-Kohn-Sham calculation that uses high-quality basis sets and hybrid exchange-correlation functional. The dual-level approach proposed by Nakajima and Hirao underlies the present method, estimating high-level four-component DFT energy perturbatively from reference density matrix, which is determined by a relatively inexpensive self-consistent calculation using low-quality basis sets and low-cost functional. A further approximation based on Infinite-Order Two-Component relativistic Hamiltonian is incorporated into the low-level treatment. Accuracy and efficiency were examined by benchmark calculation of spectroscopic values for MH, M2 (M = Cu, Ag, and Au), and AtH.

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U2 - 10.1016/j.cplett.2011.04.031

DO - 10.1016/j.cplett.2011.04.031

M3 - Article

AN - SCOPUS:79955709144

VL - 508

SP - 177

EP - 181

JO - Chemical Physics Letters

JF - Chemical Physics Letters

SN - 0009-2614

IS - 1-3

ER -