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Register a new userExperimental evidence of a collinear antiferromagnetic ordering in the frustrated CoAl2O4 spinel
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Nuclear magnetic resonance (NMR), neutron diffaction (ND), x-ray diffraction, magnetic susceptibility and specific heat measurements on the frustrated A-site spinel CoAl2O4 compound reveal a collinear antiferromagnetic ordering below Tn = 9.8(2) K. A high quality powder sample characterized by x-ray diffraction that indicates a relatively low Co-Al inversion parameter x = 0.057(20) in (Co1-xAlx)[Al2-xCox]O4, shows a broad maximum around 15 K in magnetic susceptibility and a sharp peak at Tn in heat capacity. The average ordered magnetic moment of Co^2+ (S = 3/2) ions at the A-site is estimated to be 2.4(1) Bohr magneton from NMR and 1.9(5) Bohr magneton from ND which are smaller than the expected value of 3 Bohr magneton for S = 3/2 and g = 2. Antiferromagnetic spin uctuations and correlations in the paramagnetic state are revealed from the magnetic susceptibility, NMR and ND measurements, which are due to spin frustration and site inversion effects in the system. The ND data also show short-range dynamic magnetic ordering that persists to a temperature that is almost twice Tn.
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The ground state of the frustrated A-site magnetic spinel CoAl2O4 has been a controversial issue whether it is a collinear antiferromagnetic ordering or a spiral spin - liquid state, as the ratio of the two competing interactions, J2/J1 lies close to the boundary between these two ground states. Here, we address the magnetic ground state in CoAl2O4 with different amount of Co2+/Al3+ site disorder from the study of magnetoelectric effect and Monte Carlo simulations. CoAl2O4 with low site disorder exhibits linear magnetoelectric effect below the magnetic ordering temperature. With increasing disorder, the magnetoelectric effect is suppressed and the sample with 14% disorder exhibits a spin glass behavior without the magnetoelectric effect. Monte Carlo simulations support the experimental findings and suggest that the site disorder suppresses long - range antiferromagnetic order and induces a spin glass state. Since the linear magnetoelectric effect requires a long - range magnetic ordering, we suggest that the ground state of CoAl2O4 with low site disorder is a collinear antiferromagnet.
The inversion and volume effects on magnetism in a spinel-type magnetically frustrated compound, CoAl2O4, and its gallium-substituted system, CoAl2-xGaxO4, were investigated. Magnetically frustrated Co2+ with spin S = 3/2 on the tetrahedral site formed a diamond lattice in CoAl2O4 located in the vicinity of the magnetic phase boundary between Neel and spin-spiral states. In the Ga-substituted system, the number of Co ions, the so-called inversion h dominating the octahedral site, increased with increasing x. From comprehensive crystallographic, magnetic, and thermal measurements, increments of both volume and inversion strongly reduced the Neel point, while the latter also induced a spin-glass state above the critical value of hc = 0.09. In the spin glass state, h > hc, the orbital degree of freedom of Co2+ ions in the octahedral site appeared in the magnetic entropy, which couples strongly with that of spin, even above the magnetic transitions. Above h ~ hc, the field-induced quenched magnetic moment appeared above the transitions. Therefore, a short range ordered state emerged among the paramagnetic, antiferromganetic, and spin-glass states in the magnetic phase diagram.
muSR experiments on the geometrically frustrated spinel oxide, Li2Mn2O4, show the development of spin correlations over a range of length scales with decreasing temperature. Increased relaxation below 150 K is consistent with the onset of spin correlations. Below 50 K, spin order on a length scale, which is long range for the muSR probe, appears abruptly in temperature, consistent with prior neutron diffraction results. The oscillations in the zero field asymmetry are analyzed using a three frequency model. By locating the muon site this is shown to be consistent with the unexpected 2D q = root 3 x root 3 structure on the Kagome planes proposed originally from neutron data. Longitudinal field data demonstrate that some spin dynamics persist even at 2 K. Thus, a very complex magnetic ground state, featuring the co-existence of long length scale 2D ordering and significant spin dynamics, is proposed. This is unusual considering the 3D topology of the Mn3+ spins in this material.
The crossover from localized- to itinerant-electron behavior is associated with many intriguing phenomena in condensed-matter physics. In this paper, we investigate the crossover from localized to itinerant regimes in the spinel system Mn$_{1-x}$Co$_x$V$_2$O$_4$. At low Co doping, orbital order (OO) of the localized electrons on the V3+ ions suppresses magnetic frustration by triggering a tetragonal distortion. With Co doping, electronic itinerancy melts the OO and suppresses the structural phase transition while the reduced spin-lattice coupling produces magnetic frustration. Neutron scattering measurements and first-principles-guided spin models reveal that the non-collinear state at high Co doping is produced by weakened local anisotropy and enhanced Co-V spin interactions.
We study spin liquid in the frustrated diamond lattice antiferromagnet CoAl2O4 by means of single crystal neutron scattering in zero and applied magnetic field. The magnetically ordered phase appearing below TN=8 K remains nonconventional down to 1.5 K. The magnetic Bragg peaks at the q=0 positions remain broad and their profiles have strong Lorentzian contribution. Additionally, they are connected by weak diffuse streaks along the <111> directions. These observations are explained within the spiral spin liquid model as short-range magnetic correlations of spirals populated at these finite temperatures, as the energy minimum around q=0 is flat and the energy of excited states with q=(111) is low. The agreement is only qualitative, leading us to suspect that microstructure effects are also important. Magnetic field significantly perturbs spin correlations. The 1.5 K static magnetic moment increases from 1.58 mB/Co at zero field to 2.08 mB/Co at 10 T, while the magnetic peaks, being still broad, acquire almost Gaussian profile. Spin excitations are rather conventional spin waves at zero field, resulting in the exchange parameters J1=0.92(1) meV, J2=0.101(2) meV and the anisotropy term D=-0.0089(2) meV for CoAl2O4. The application of a magnetic field leads to a pronounced broadening of the excitations at the zone center, which at 10 T appear gapless and nearly featureless.
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