Title: Importance of charge self-consistency in first-principles description of strongly correlated systems

Journal Article · · npj Computational Materials
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1];  [3]; ORCiD logo [1]
  1. Radboud Univ., Nijmegen (The Netherlands)
  2. King’s College London (United Kingdom)
  3. King’s College London (United Kingdom); National Renewable Energy Lab. (NREL), Golden, CO (United States)
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First-principles approaches have been successful in solving many-body Hamiltonians for real materials to an extent when correlations are weak or moderate. As the electronic correlations become stronger often embedding methods based on first-principles approaches are used to better treat the correlations by solving a suitably chosen many-body Hamiltonian with a higher level theory. The success of such embedding theories, often referred to as second-principles, is commonly measured by the quality of self-energy Σ which is either a function of energy or momentum or both. However, Σ should, in principle, also modify the electronic eigenfunctions and thus change the real space charge distribution. While such practices are not prevalent, some works that use embedding techniques do take into account these effects. In such cases, choice of partitioning, of the parameters defining the correlated Hamiltonian, of double-counting corrections, and the adequacy of low-level Hamiltonian hosting the correlated subspace hinder a systematic and unambiguous understanding of such effects. Further, for a large variety of correlated systems, strong correlations are largely confined to the charge sector. Then an adequate nonlocal low-order theory is important, and the high-order local correlations embedding contributes become redundant. Here we study the impact of charge self-consistency within two example cases, TiSe2 and CrBr3, and show how real space charge re-distribution due to correlation effects taken into account within a first-principles Green’s function-based many-body perturbative approach is key in driving qualitative changes to the final electronic structure of these materials.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1839380
Report Number(s):
NREL/JA-5F00-81840; MainId:82613; UUID:92776787-187b-4a58-af09-6e672fbd1661; MainAdminID:63581
Journal Information:
npj Computational Materials, Journal Name: npj Computational Materials Journal Issue: 1 Vol. 7; ISSN 2057-3960
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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