TY - JOUR
T1 - Electronic properties of RX2Al20 (R = La, Ce, Yb, Th, U; X = Ti, V, Cr and Mn) cage compounds
AU - Swatek, Przemysław
AU - Kleinert, Maja
AU - Wiśniewski, Piotr
AU - Kaczorowski, Dariusz
N1 - Publisher Copyright:
© 2018 Elsevier B.V.
PY - 2018/10
Y1 - 2018/10
N2 - Non-spin-polarized electronic structures and Fermi surface properties of RX2Al20 (R = La, Ce, Yb, Th, U; X = Ti, V, Cr, Mn) intermetallic compounds were calculated using the full potential all-electron local orbital (FPLO) approach in the framework of the local density approximation (LDA). Trends of the magnetism are discussed in terms of the characteristics of X-3d bands with a quantitative analysis of the relationship between band electron filling and crystal electric field splitting. Since coordination icosahedra of X-atoms have small trigonal distortion, crystal electric field splits the fivefold degenerate X-3d state into low-energy singlet a1g and two higher-energy doublets eg. In RTi2Al20 and RV2Al20 the population of the related 3d sub-band is not sufficient to cause energetically favorable spin polarization, whereas magnetic instabilities develop in the RCr2Al20 series. Finally, a manifestation of strong repulsive interactions between itinerant Mn-d electrons become most pronounced in ferromagnetic UMn2Al20. The influence of non-magnetic R-f states on magnetic and thermodynamic properties is discussed with special emphasis on the role of the f–p and f–d hybridization. For LaTi2Al20 and LaV2Al20 the calculated quantum oscillation frequencies are in accord with experimental reports.
AB - Non-spin-polarized electronic structures and Fermi surface properties of RX2Al20 (R = La, Ce, Yb, Th, U; X = Ti, V, Cr, Mn) intermetallic compounds were calculated using the full potential all-electron local orbital (FPLO) approach in the framework of the local density approximation (LDA). Trends of the magnetism are discussed in terms of the characteristics of X-3d bands with a quantitative analysis of the relationship between band electron filling and crystal electric field splitting. Since coordination icosahedra of X-atoms have small trigonal distortion, crystal electric field splits the fivefold degenerate X-3d state into low-energy singlet a1g and two higher-energy doublets eg. In RTi2Al20 and RV2Al20 the population of the related 3d sub-band is not sufficient to cause energetically favorable spin polarization, whereas magnetic instabilities develop in the RCr2Al20 series. Finally, a manifestation of strong repulsive interactions between itinerant Mn-d electrons become most pronounced in ferromagnetic UMn2Al20. The influence of non-magnetic R-f states on magnetic and thermodynamic properties is discussed with special emphasis on the role of the f–p and f–d hybridization. For LaTi2Al20 and LaV2Al20 the calculated quantum oscillation frequencies are in accord with experimental reports.
KW - Caged compounds
KW - Electronic band calculations
KW - Fermi surface
KW - Orbital hybridization
KW - Quantum oscillations
KW - Rare earth intermetallics
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U2 - 10.1016/j.commatsci.2018.06.047
DO - 10.1016/j.commatsci.2018.06.047
M3 - Article
AN - SCOPUS:85049915891
SN - 0927-0256
VL - 153
SP - 461
EP - 472
JO - Computational Materials Science
JF - Computational Materials Science
ER -