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Ab Initio Full Cell GW+DMFT for Correlated Materials

Zhu, Tianyu and Chan, Garnet Kin-Lic (2021) Ab Initio Full Cell GW+DMFT for Correlated Materials. Physical Review X, 11 (2). Art. No. 021006. ISSN 2160-3308. doi:10.1103/PhysRevX.11.021006.

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The quantitative prediction of electronic properties in correlated materials requires simulations without empirical truncations and parameters. We present a method to achieve this goal through a new ab initio formulation of dynamical mean-field theory (DMFT). Instead of using small impurities defined in a low-energy subspace, which require complicated downfolded interactions which are often approximated, we describe a full cell GW+DMFT approach, where the impurities comprise all atoms in a unit cell or supercell of the crystal. Our formulation results in large impurity problems, which we treat here with efficient quantum chemistry impurity solvers that work on the real-frequency axis, combined with a one-shot G₀W₀ treatment of long-range interactions. We apply our full cell approach to bulk Si, two antiferromagnetic correlated insulators NiO and α−Fe₂O₃, and the paramagnetic correlated metal SrMoO₃, with impurities containing up to ten atoms and 124 orbitals. We find that spectral properties, magnetic moments, and two-particle spin correlation functions are obtained in good agreement with experiment. In addition, in the metal oxide insulators, the balanced treatment of correlations involving all orbitals in the cell leads to new insights into the orbital character around the insulating gap.

Item Type:Article
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URLURL TypeDescription Paper
Zhu, Tianyu0000-0003-2061-3237
Chan, Garnet Kin-Lic0000-0001-8009-6038
Additional Information:© 2021 Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI. Received 7 March 2020; revised 13 November 2020; accepted 4 January 2021; published 6 April 2021. This work was supported by the U.S. Department of Energy via the M²QM EFRC under Grant No. de-sc0019330. We thank Cyrus Umrigar and Yuan Yao for providing the SHCI Green’s function code. T. Z. thanks Zhihao Cui, Xing Zhang, and Timothy Berkelbach for helpful discussions. Additional support was provided by the Simons Foundation via the Simons Collaboration on the Many Electron Problem and via the Simons Investigatorship in Physics.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0019330
Simons FoundationUNSPECIFIED
Issue or Number:2
Record Number:CaltechAUTHORS:20200420-105853289
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:102652
Deposited By: Tony Diaz
Deposited On:20 Apr 2020 19:01
Last Modified:21 Apr 2021 17:11

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