An unusual orbital state was recently proposed to explain the magnetic and transport properties of Ba$_3$CoRu$_2$O$_9$ [Phys. Rev. B. {\bf 85}, 041201 (2012)]. We show that this state contradicts to the first Hund's rule and does not realize in the system under consideration because of a too small crystal-field splitting in the $t_{2g}$ shell. A strong suppression of the local magnetic moment in Ba$_3$CoRu$_2$O$_9$ is attributed to a strong hybridization between the Ru 4$d$ and O 2$p$ states.
We elucidate the microscopic mechanism that causes a suppression of ferroelectricity and an enhancement of octahedral rotations in EuTiO3 from first principles. We find that the hybridization of the rare-earth Eu 4f states with the B-site Ti cation drives the system away from ferroelectricity. We also show that the magnetic order dependence of this hybridization is the dominant source of spin-phonon coupling in this material. Our results underline the importance of rare-earth f electrons on the lattice dynamics and stability of these transition metal oxides.
The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the magnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is nec…
We show for the system La1-xCexCoO3 (0.1 <= x <= 0.4) that it is possible to synthesize electron-doped cobaltites by the growth of epitaxial thin films. For La1-xCexCoO3, ferromagnetic order is observed within the entire doping range (with the maximum of the Curie temperature, Tc, at x ca. 0.3), resulting in a magnetic phase diagram similar to that of hole-doped lanthanum cobaltites. The measured spin values strongly suggest an intermediate-spin state of the Co ions which has been also found in the hole-doped system. In contrast to the hole-doped material, however, where Tc is well above 200 K…
Among the members of the series R2PdSi3 (R= Rare-earths), the magnetic behavior of the Nd compound is interesting in some respects. This compound is considered to order ferromagnetically (below 16 K), unlike other members of this series which order antiferromagnetically. In addition, magnetic ordering temperature (To) is significantly enhanced with respect to de Gennes scaled value. In order to understand the magnetism of this compound better, we have investigated the magnetic behavior in detail (under external pressure as well) and also of its solid solutions based on substitutions at Nd and …
The intermediate valence compound YbAl3 exhibits a broad magnetic excitation with characteristic energy E1 ~ 50meV, of order of the Kondo energy (TK ~ 600-700K). In the low temperature (T < Tcoh ~ 40K) Fermi liquid state, however, a new magnetic excitation arises at E2 ~ 33meV, which lies in the hybridization gap that exists in this compound. We show, using inelastic neutron scattering on a single-crystal sample, that while the scattering at energies near E1 has the momentum (Q-) dependence expected for interband scattering across the indirect gap, the scattering near E2 is independent of Q. T…
Momentum-transfer (q) dependent non-resonant inelastic x-ray scattering measurements were made at the N4,5 edges for several rare earth compounds. With increasing q, giant dipole resonances diminish, to be replaced by strong multiplet lines at lower energy transfer. These multiplets result from two different orders of multipole scattering and are distinct for systems with simple 4f^0 and 4f^1 initial states. A many-body theoretical treatment of the multiplets agrees well with the experimental data on ionic La and Ce phosphate reference compounds. Comparing measurements on CeO2 and CeRh3 to the…
The recent discovery of topological Kondo insulating behaviour in strongly correlated electron systems has generated considerable interest in Kondo insulators both experimentally and theoretically. The Kondo semiconductors CeT2Al10 (T=Fe, Ru and Os) possessing a c-f hybridization gap have received considerable attention recently because of the unexpected high magnetic ordering temperature of CeRu2Al10 (TN=27 K) and CeOs2Al10 (TN=28.5 K) and the Kondo insulating behaviour observed in the valence fluctuating compound CeFe2Al10 with a paramagnetic ground state down to 50 mK. We are investigating …
Magnetism in monolayer (ML) VSe2 has attracted broad interest in spintronics while existing reports have not reached consensus. Using element-specific X-ray magnetic circular dichroism, a magnetic transition in ML VSe2 has been demonstrated at the contamination-free interface between Co and VSe2. Via interfacial hybridization with Co atomic overlayer, a magnetic moment of about 0.4 uB per V atom in ML VSe2 is revealed, approaching values predicted by previous theoretical calculations. Promotion of the ferromagnetism in ML VSe2 is accompanied by its antiferromagnetic coupling to Co and a reduct…
We theoretically and numerically show that longitudinal orbital currents in ferromagnets depend on the magnetization direction, which contribute to the anisotropic magnetoresistance (AMR). This orbital contribution to AMR arises from the momentum-dependent orbital splitting, which is generally present in multi-orbital systems through the orbital anisotropy and the orbital hybridization. We highlight the latter orbital hybridization as an unrecognized origin of AMR and also as a common origin of AMR and orbital Hall effect.
We present the cationic impurity assisted band offset phenomena in NixCd1-xO (x= 0, 0.02, 0.05, 0.1, 0.2, 0.4, 0.8, 1) thin films and further discussed in the light of orbital hybridization modification. Compositional and structural studies revealed that cationic substitution of Cd2+ by Ni2+ ions leads to a monotonic shift in (220) diffraction peak, indicating the suppression of lattice distortion while evolution of local strain with increasing Ni concentration mainly associated to the mismatch in electro-negativity of Cd2+ and Ni2+ ion. In fact, Fermi level pinning towards conduction band min…
The discovery of unconventional superconductivity in hole doped NdNiO2, similar to CaCuO2, has received enormous attention. However, different from CaCuO2, RNiO2 (R = Nd, La) has itinerant electrons in the rare-earth spacer layer. Previous studies show that the hybridization between Ni-dx2-y2 and rare-earth-d orbitals is very weak and thus RNiO2 is still a promising analog of CaCuO2. Here, we perform first-principles calculations to show that the hybridization between Ni-dx2-y2 orbital and itinerant electrons in RNiO2 is substantially stronger than previously thought. The dominant hybridizatio…
The plasmonic character of monolayer silicene is investigated by time-dependent density functional theory in the random phase approximation. The energy-loss function of the system is analyzed, with particular reference to its induced charge-density fluctuations, i.e., plasmon resonances and corresponding dispersions, occurring in the investigated energy-momentum region. At energies larger than 1.5eV, two intrinsic interband modes are detected and characterized. The first one is a hybridized pi-like plasmon, which is assisted by competing one-electron processes involving sp2 and sp3 states. The…
Artificially fabricated 3$d$/5$d$ superlattices (SLs) involve both strong electron correlation and spin-orbit coupling in one material by means of interfacial 3$d$-5$d$ coupling, whose mechanism remains mostly unexplored. In this work we investigated the mechanism of interfacial coupling in LaMnO$_3$/SrIrO$_3$ SLs by several spectroscopic approaches. Hard x-ray absorption, magnetic circular dichroism and photoemission spectra evidence the systematic change of the Ir ferromagnetism and the electronic structure with the change of the SL repetition period. First-principles calculations further re…
Nanoscale CeO2 (nanoceria) is a prototypical system that presents d0 ferromagnetism. Using a combination of x-ray absorption spectroscopy, x-ray magnetic circular dichroism and modelling, we show that nanostructure, defects and disorder, and non-stoichiometry create magnetically polarized Ce 4f and O 2p hybridized states captured by the vacancy orbitals (Vorb) that are vital to ferromagnetism. Further, we demonstrate that foreign ions (Fe and Co) enhance the moment at Ce 4f sites while the number of Vorb is unchanged, pointing clearly to the mechanism of orbital hybridization being key missing…
We have investigated the impact of covalent hybridization on martensitic structure and magnetic properties of Ni50Mn5+xGa35-xCu10 shape memory alloys. We found that the lattice distortion ((c-a)/a) of L10 martensite monotonously changes with the substitution of Mn for Ga atoms and shows a kink behavior at Ga(at.%)= 25 due to the weakened covalent effect between main-group and transition-metal atoms. Moreover, owing to the competition between covalence hybridization and magnetic ordering of introduced Mn atoms, the molecular magnetic moment and Curie temperature coincidently show maximums at Ga…
We have performed a systematic first-principles computational study of the effects of impurity atoms (boron, carbon, nitrogen, oxygen, silicon, phosporus, and sulfur) on the orbital hybridization and bonding properties in the intermetallic alloy NiAl using a full-potential linear muffin-tin orbital method. The matrix elements in momentum space were used to calculate real-space properties: onsite parameters, partial densities of states, and local charges. In impurity atoms that are empirically known to be embrittler (N and O) we found that the 2s orbital is bound to the impurity and therefore d…
From first principles calculations we unravel surprisingly strong interactions between arsenic ions in iron-pnictides, the strength of which is controlled by the Fe-spin state. Reducing the Fe-magnetic moment, weakens the Fe-As bonding, and in turn, increases As-As interactions, causing giant reduction in the c-axis. For CaFe$_2$As$_2$ system, this reduction is as large as 1.4 Å. Since the large c-reduction has been recently observed only under high-pressure\cite{cTphase}, our results suggest that the iron magnetic moment should be present in Fe-pnictides at all times at ambient pressure. Fina…
The magnetic-field dependence of many-body states in quantum dots can be tailored by controlling the mixing of various angular momenta. In lateral quantum dots -- defined electrostatically in a two-dimensional electron gas -- this mixing can be accomplished by introducing anisotropies in the confinement potential, thereby explicitly breaking rotational symmetry. Mixing can be severe enough to violate Hund's rules, even at zero magnetic field. We illustrate the principle through calculations of states and spectra of four-electron droplets (p-shell) with long-range Coulomb repulsions and confine…
