Maximilian E. Merkel^1*, Aria Mansouri Tehrani^1,2, Claude Ederer^1*

1 Materials Theory, ETH Zürich, 8093 Zürich, Switzerland

2 Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

* Corresponding authors emails: maximilian.merkel@mat.ethz.ch, claude.ederer@mat.ethz.ch

DOI10.24435/materialscloud:24-a9 [version v1]

Publication date: Feb 22, 2024

How to cite this record

Maximilian E. Merkel, Aria Mansouri Tehrani, Claude Ederer, Probing the Mott-insulating behavior of Ba₂MgReO₆ with DFT+DMFT, Materials Cloud Archive 2024.36 (2024), https://doi.org/10.24435/materialscloud:24-a9

Description

We investigate the interplay of spin-orbit coupling, electronic correlations, and lattice distortions in the 5d¹ double perovskite Ba₂MgReO₆. Combining density-functional theory (DFT) and dynamical mean-field theory (DMFT), we establish the Mott-insulating character of Ba₂MgReO₆ in both its cubic and tetragonal paramagnetic phases. Despite substantial spin-orbit coupling, its impact on the formation of the insulating state is minimal, consistent with theoretical expectations for d¹ systems. We further characterize the electronic properties of the cubic and tetragonal phases by analyzing spectral functions and local occupations in terms of multipole moments centered on the Re sites. Our results confirm the presence of ferroically ordered z² quadrupoles in addition to the antiferroic x²-y²-type order. We compare two equivalent but complementary descriptions in terms of either effective Re-t2g frontier orbitals or more localized atomic-like Re-d and O-p orbitals. The former maps directly on a physically intuitive picture in terms of nominal d¹ Re cations, while the latter explicitly demonstrates the role of hybridization with the ligands in the spin-orbit splitting and the formation of the charge quadrupoles around the Re sites. Finally, we compare our DFT+DMFT results with a previous DFT+U study of the tetragonal paramagnetic state. We find good qualitative agreement for the dominant charge quadrupoles, but also notable differences in the corresponding spectral functions, underscoring the need for more comparative studies between these two methods.

Materials Cloud sections using this data

Files

File name	Size	Description
README.md MD5md5:71af4ad03aa84f53c5b9aaf5d85b4e85	4.5 KiB	Description of the contents of the accompanying .tar.gz archives and short instructions on DFT and DMFT workflow
data.tar.gz MD5md5:f4e1e2222ebddab95774f0e58900b118	2.8 GiB	tar.gz archive with all our data and scripts
data_dft_para_rand.tar.gz MD5md5:9375b91a4301058e16a6f1995aa3b88f	40.4 MiB	DFT+U data from doi.org/10.1103/PhysRevMaterials.5.104410 used to compare to our data
solid_dmft_soc_real.tar.gz MD5md5:e4012142e27e1d20aa8a1a415415cebd	99.2 KiB	solid_dmft code used for calculations, including the modifications for spin-orbit coupling
dmft_projectors.tar.gz MD5md5:6f83210d45377057f3e6a39ad6f0e2aa	1.5 KiB	python scripts used for different projectors

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External references

Keywords

double perovskite Mott insulator dynamical mean-field theory density-functional theory constrained random-phase approximation