Incorporating static intersite correlation effects in vanadium dioxide through DFT+V
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Date
2024
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Journal Article
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Abstract
We analyze the effects on the structural and electronic properties of vanadium dioxide (VO2) due to adding an empirical interatomic potential within the density-functional theory + V (DFT + V ) framework. We use the DFT + V machinery founded on the extended Hubbard model to apply an empirical self-energy correction between nearest-neighbor vanadium atoms in both rutile and monoclinic phases, and for a set of structures interpolating between these two cases. We observe that imposing an explicit intersite interaction V along the vanadium–vanadium chains enhances the characteristic bonding-antibonding splitting of the relevant bands in the monoclinic phase, thus favoring electronic dimerization and the formation of a bandgap. We then explore the effect of V on the structural properties and the relative energies of the two phases, finding an insulating global energy minimum for the monoclinic phase, consistent with experimental observations. With increasing V , this
minimum becomes deeper relative to the rutile structure, and the transition from the metallic to the insulating state becomes sharper. We also analyze the effect of applying the +V correction either to all or only to selected vanadium–vanadium pairs and both in the monoclinic as well as the metallic rutile phase. Our results suggest that DFT + V can indeed serve as a computationally inexpensive unbiased way of modeling VO2 which is well suited for studies that, e.g., require large system sizes.
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published
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6 (4)
Pages / Article No.
43177
Publisher
American Physical Society
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03903 - Spaldin, Nicola A. / Spaldin, Nicola A.
Notes
Funded through the Swiss National Science Foundation Grant: CRSII5_209454 „Neuromimetic metal-oxide memristors (NeMO)"