Altermagnetic (AM) materials exhibit non-relativistic, momentum-dependent spin-split states, ushering in new opportunities for spin electronic devices. While the characteristics of spin-splitting are documented within the framework of the non-relativistic spin group symmetry, there is limited exploration of the inclusion of relativistic symmetry and its impact on the emergence of a novel spin-splitting in the band structure. This study delves into the intricate relativistic electronic structure of an AM material, α-MnTe. Employing temperature-dependent angle-resolved photoelectron spectroscopy across the AM phase transition, the emergence of a relativistic valence band splitting concurrent with the establishment of magnetic order is elucidated. This discovery is validated through disordered local moment calculations, modeling the influence of magnetic order on the electronic structure and confirming the magnetic origin of the observed splitting. The temperature-dependent splitting is ascribed to the advent of relativistic spin-splitting resulting from the strengthening of AM order in α-MnTe as the temperature decreases. This sheds light on a previously unexplored facet of this intriguing material.
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http://dx.doi.org/10.1002/adma.202314076 | DOI Listing |
J Chem Theory Comput
December 2024
Fundamental Science Center of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China.
Relativistic pseudopotentials (PPs) and basis sets are the workhorses for modeling heavy elements of lanthanides and actinides. The norm-conserving Goedecker-Teter-Hutter (GTH) PP is advantageous for modeling lanthanide and actinide compounds and condensed systems because of its transferability and accuracy. In this work, we develop a set of well-benchmarked GTH-type 5f-in-core PPs with scalar-relativistic effects together with associated Gaussian basis sets for the most commonly encountered trivalent and tetravalent actinides [An(III), An(IV); An = Pa-Lr].
View Article and Find Full Text PDFJ Chem Theory Comput
November 2024
Department of Chemistry and Molecular Physics, São Carlos Institute of Chemistry, University of São Paulo, C.P. 780, São Carlos, São Paulo 13560-970, Brazil.
This study presents two new relativistic Gaussian basis sets without variational prolapse of double- and triple-ζ quality, RPF-2Z and RPF-3Z, along with augmented versions including additional diffuse functions, aug-RPF-2Z and aug-RPF-3Z, which are available for all and block elements from Hydrogen to Oganesson. The exponents of the Correlation/Polarization (C/P) functions are obtained from a polynomial version of the generator coordinate Dirac-Fock method (p-GCDF). The choice of C/P functions was guided by multireference configuration interaction calculations with single and double excitations (MR-CISD) based on a valence active space.
View Article and Find Full Text PDFJ Phys Chem A
November 2024
Chair of Theoretical Chemistry, Department of Chemistry, Ludwig-Maximilians-Universität München, Butenandtstr. 5-13, Munich D-81377, Germany.
Sci Rep
October 2024
IT4Innovations and Nanotechnology Centre, CEET, VSB-Technical University of Ostrava, 17. listopadu 2172/15, 70800, Ostrava, Czech Republic.
Correlated band theory implemented as a combination of the relativistic density functional theory with exact diagonalization [DFT+U(ED)] of the Anderson impurity term with Coulomb repulsion U in the 5f shell is applied to the magnetic field polarized state of [Formula: see text]. We demonstrate that the DFT+U(ED) approach provides a good agreement with very recent x-ray absorbtion near edge structure (XANES) and x-ray magnetic circular dichroism (XMCD) experiments. The branching ratio for the [Formula: see text] edge transitions of uranium, and the valence spin-orbit interaction per hole were evaluated in a perfect agreement with the XANES.
View Article and Find Full Text PDFFront Chem
September 2024
GSI Helmholtzzentrum für Schwerionenforschung, Darmstadt, Germany.
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