No Arabic abstract
Compounds based on the Fe2P structure have continued to attract interest because of the interplay between itinerant and localized magnetism in a non-centrosymmetric crystal structure, and because of the recent developments of these materials for magnetocaloric applications. Here we report the growth and characterization of mm size single crystals of FeMnP0.8Si0.2. Single crystal x-ray diffraction, magnetization, resistivity, Hall and heat capacity data are reported. Surprisingly, the crystals exhibit itinerant antiferromagnetic order below 158 K with no hint of ferromagnetic behavior in the magnetization curves and with the spins ordered primarily in the ab plane. The room temperature resistivity is close to the Ioffe-Regel limit for a metal. Single crystal x-ray diffraction indicates a strong preference for Mn to occupy the larger pyramidal 3g site. The cation site preference in the as-grown crystals and the antiferromagnetism are not changed after high temperature anneals and a rapid quench to room temperature.
Crystallographic, electronic transport, thermal and magnetic properties are reported for SrMn2As2 and CaMn2As2 single crystals grown using Sn flux. Rietveld refinements of powder x-ray diffraction data show that the two compounds are isostructural and crystallize in the trigonal CaAl2Si2-type structure (space group P-3m1), in agreement with the literature. Electrical resistivity rho versus temperature T measurements demonstrate insulating ground states for both compounds with activation energies of 85 meV for SrMn2As2 and 61 meV for CaMn2As2. In a local-moment picture, the Mn^{+2} 3d^5 ions are expected to have high-spin S = 5/2 with spectroscopic splitting factor g = 2. Magnetic susceptibility chi and heat capacity measurements versus T reveal antiferromagnetic (AFM) transitions at TN = 120(2) K and 62(3) K for SrMn2As2 and CaMn2As2, respectively. The anisotropic chi(T < TN) data indicate that the hexagonal c axis is the hard axis and hence that the ordered Mn moments are aligned in the ab plane. The chi(T) for both compounds and Cp(T) data for SrMn2As2 show strong dynamic short-range AFM correlations from TN up to at least 900 K, likely associated with quasi-two-dimensional connectivity of strong AFM exchange interactions between the Mn spins within the corrugated honeycomb Mn layers parallel to the ab plane.
Identifying the nature of magnetism, itinerant or localized, remains a major challenge in condensed-matter science. Purely localized moments appear only in magnetic insulators, whereas itinerant moments more or less co-exist with localized moments in metallic compounds such as the doped-cuprate or the iron-based superconductors, hampering a thorough understanding of the role of magnetism in phenomena like superconductivity or magnetoresistance. Here we distinguish two antiferromagnetic modulations with respective propagation wave vectors of $Q_{pm}$ = ($H pm 0.557(1)$, 0, $L pm 0.150(1)$) and $Q_text{C}$ = ($H pm 0.564(1)$, 0, $L$), where $left(H, Lright)$ are allowed Miller indices, in an ErPd$_2$Si$_2$ single crystal by neutron scattering and establish their respective temperature- and field-dependent phase diagrams. The modulations can co-exist but also compete depending on temperature or applied field strength. They couple differently with the underlying lattice albeit with associated moments in a common direction. The $Q_{pm}$ modulation may be attributed to localized 4emph{f} moments while the $Q_text{C}$ correlates well with itinerant conduction bands, supported by our transport studies. Hence, ErPd$_2$Si$_2$ represents a new model compound that displays clearly-separated itinerant and localized moments, substantiating early theoretical predictions and providing a unique platform allowing the study of itinerant electron behavior in a localized antiferromagnetic matrix.
FeGe_2, and lightly doped compounds based on it, have a Fermi surface driven instability which drive them into an incommensurate spin density wave state. Studies of the temperature and magnetic field dependence of the resistivity have been used to determine the magnetic phase diagram of the pure material which displays an incommensurate phase at high temperatures and a commensurate structure below 263 K in zero field. Application of a magnetic field in the tetragonal basal plane decreases the range of temperatures over which the incommensurate phase is stable. We have used inelastic neutron scattering to measure the spin dynamics of FeGe_2. Despite the relatively isotropic transport the magnetic dynamics is quasi-one dimensional in nature. Measurements carried out on HET at ISIS have been used to map out the spin wave dispersion along the c-axis up the 400 meV, more than an order of magnitude higher than the zone boundary magnon for wavevectors in the basal plane.
Susceptibility, specific heat, and muon spin rotation measurements on high-quality single crystals of $rm Na_{0.82}CoO_2$ have revealed bulk antiferromagnetism with N{e}el temperature $rm T_N = 19.8 pm 0.1$ K and an ordered moment perpendicular to the $rm CoO_2$ layers. The magnetic order encompasses nearly 100% of the crystal volume. The susceptibility exhibits a broad peak around 30 K, characteristic of two-dimensional antiferromagnetic fluctuations. The in-plane resistivity is metallic at high temperatures and exhibits a minimum at $rm T_N$.
Bulk rutile RuO$_2$ has long been considered a Pauli paramagnet. Here we report that RuO$_2$ exhibits a hitherto undetected lattice distortion below approximately 900 K. The distortion is accompanied by antiferromagnetic order up to at least 300 K with a small room temperature magnetic moment of approximately 0.05 $mu_B$ as evidenced by polarized neutron diffraction. Density functional theory plus $U$ (DFT+$U$) calculations indicate that antiferromagnetism is favored even for small values of the Hubbard $U$ of the order of 1 eV. The antiferromagnetism may be traced to a Fermi surface instability, lifting the band degeneracy imposed by the rutile crystal field. The combination of high Neel temperature and small itinerant moments make RuO$_2$ unique among ruthenate compounds and among oxide materials in general.