DMRG on Top of Plane-Wave Kohn-Sham Orbitals: A Case Study of Defected Boron NitrideShow others and affiliations
2021 (English)In: Journal of Chemical Theory and Computation, ISSN 1549-9618, E-ISSN 1549-9626, Vol. 17, no 2, p. 1143-1154Article in journal (Refereed) Published
Abstract [en]
In this paper, we analyze the numerical aspects of the inherent multireference density matrix renormalization group (DMRG) calculations on top of the periodic Kohn-Sham density functional theory using the complete active space approach. The potential of the framework is illustrated by studying hexagonal boron nitride nanoflakes embedding a charged single boron vacancy point defect by revealing a vertical energy spectrum with a prominent multireference character. We investigate the consistency of the DMRG energy spectrum from the perspective of sample size, basis size, and active space selection protocol. Results obtained from standard quantum chemical atom-centered basis calculations and plane-wave based counterparts show excellent agreement. Furthermore, we also discuss the spectrum of the periodic sheet which is in good agreement with extrapolated data of finite clusters. These results pave the way toward applying the DMRG method in extended correlated solid-state systems, such as point defect qubit in wide band gap semiconductors.
Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2021. Vol. 17, no 2, p. 1143-1154
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-174389DOI: 10.1021/acs.jctc.0c00809ISI: 000634678200045PubMedID: 33435672OAI: oai:DiVA.org:liu-174389DiVA, id: diva2:1538742
Note
Funding Agencies|NKFIH [PD-17-125261, FK-20-135496, K120569, K134983]; Bolyai Research Scholarship of the Hungarian Academy of SciencesHungarian Academy of Sciences; MTA Premium Postdoctoral Research Program; Knut and Alice Wallenberg Foundation through WBSQD2 project [2018.0071]; Czech Science FoundationGrant Agency of the Czech Republic [18-18940Y]; NKFIH through the National Quantum Technology Program [2017-1.2.1-NKP-2017-00001]; Alexander von Humboldt FoundationAlexander von Humboldt Foundation; Hungarian NKFIH of the National Excellence Program of the Quantum-coherent materials project [KKP129866]; Center for Scalable and Predictive methods for Excitation and Correlated phenomena (SPEC) from the Computational Chemical Sciences Program by the U.S. Department of Energy (DOE), at the Pacific Northwest National LaboratoryUnited States Department of Energy (DOE)
2021-03-212021-03-212024-01-10