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Register a new userAnomalous spin-waves and the commensurate-incommensurate magnetic phase transition in LiNiPO4
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Thomas Bagger Stibius Jensen
Publication date
2009
fields
Physics
and research's language is
English
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Detailed spin-wave spectra of magneto-electric LiNiPO4 have been measured by neutron scattering at low temperatures in the commensurate (C) antiferromagnetic (AF) phase with ordering temperature 20.8 K. An anomalous low-energy mode is observed at the modulation vector of the incommensurate (IC) AF phase appearing above the 20.8 K. A linear spin-wave model based on Heisenberg exchange couplings and single ion anisotropies accounts for all the observed spin-wave dispersions and intensities. Along the b axis an unusually strong next-nearest-neighbor AF coupling competes with the dominant nearest-neighbor AF exchange interaction and causes the IC structure.
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We have performed simultaneous measurements of magnetic chirality by using polarized neutrons and electric polarization along the b-axis of single crystals of YMn$^{4+}$(Mn$_{1-x}$Ga$_{x}$)$^{3+}$O$_{5}$ with $x=0.047$ and 0.12, in which nonmagnetic Ga-ions dilute Mn$^{3+}$ spins. The $x=0.047$ sample exhibits high-temperature incommensurate (HT-ICM), commensurate (CM), and low-temperature incommensurate (LT-ICM) magnetic phases in order of decreasing temperature, whereas the $x=0.12$ sample exhibits only HT-ICM and LT-ICM phases. Here, the CM and LT-ICM phases are ferroelectric and weak-ferroelectric, respectively. Measurements conducted under zero field heating after various field-cooling conditions evidence that the microscopic mechanisms of the spin-driven ferroelectricity in the CM and LT-ICM phases are different: the magnetic chirality of Mn$^{4+}$ cycloidal spins plays a dominant role in the LT-ICM phase, whereas the magnetic exchange striction by the Mn$^{4+}$-Mn$^{3+}$ chain plays a dominant role in the CM phase. The polarization of YMn$_{2}$O$_{5}$ flips upon CM to LT-ICM phase transition because the ferroelectricity driven by the magnetic chirality and the exchange striction provides opposite directions of polarization.
We report thermodynamic properties, magnetic ground state, and microscopic magnetic model of the spin-1 frustrated antiferromaget Li$_{2}$NiW$_{2}$O$_{8}$ showing successive transitions at $T_{rm N1}simeq 18$ K and $T_{rm N2}simeq 12.5$ K in zero field. Nuclear magnetic resonance and neutron diffraction reveal collinear and commensurate magnetic order with the propagation vector $mathbf k=(frac12,0,frac12)$ below $T_{rm N2}$. The ordered moment of 1.8 $mu_B$ at 1.5 K is directed along $[0.89(9),-0.10(5),-0.49(6)]$ and matches the magnetic easy axis of spin-1 Ni$^{2+}$ ions, which is determined by the scissor-like distortion of the NiO$_6$ octahedra. Incommensurate magnetic order, presumably of spin-density-wave type, is observed in the region between $T_{rm N2}$ and $T_{rm N1}$. Density-functional band-structure calculations put forward a three-dimensional spin lattice with spin-1 chains running along the $[01bar 1]$ direction and stacked on a spatially anisotropic triangular lattice in the $ab$ plane. We show that the collinear magnetic order in Li$_2$NiW$_2$O$_8$ is incompatible with the triangular lattice geometry and thus driven by a pronounced easy-axis single-ion anisotropy of Ni$^{2+}$.
Neutron diffraction is used to probe the (H,T) phase diagram of magneto-electric (ME) LiNiPO4 for magnetic fields along the c-axis. At zero field the Ni spins order in two antiferromagnetic phases. One has commensurate (C) structures and general ordering vectors (0,0,0), the other one is incommensurate (IC) with ordering vector (0,q,0). At low temperatures the C order collapses above 12 Tesla and adopts an IC structure with modulation vector parallel to (0,q,0). We show that C order is required for the ME effect and establish how electric polarization results from a field-induced reduction of the total magneto-elastic energy.
The layered {beta}-NaMnO2, a promising Na-ion energy-storage material has been investigated for its triangular lattice capability to promote complex magnetic configurations that may release symmetry restrictions for the coexistence of ferroelectric and magnetic orders. The complexity of the neutron powder diffraction patterns underlines that the routinely adopted commensurate structural models are inadequate. Instead, a single-phase superspace symmetry description is necessary, demonstrating that the material crystallizes in a compositionally modulated q= (0.077(1), 0, 0) structure. Here, Mn3+ Jahn-Teller distorted MnO6 octahedra form corrugated layer stacking sequences of the {beta}-NaMnO2 type, which are interrupted by flat sheets of the {alpha}-like oxygen topology. Spontaneous long-range collinear antiferromagnetic order, defined by the propagation vector k= (1/2, 1/2, 1/2), appears below TN1= 200 K. Moreover, a second transition into a spatially modulated proper-screw magnetic state (k+-q) is established at TN2= 95 K, with an antiferromagnetic order parameter resembling that of a two-dimensional (2D) system. The evolution of 23Na NMR spin-lattice relaxation identifies a magnetically inhomogene-ous state in the intermediate T-region (TN2 <T< TN1), while its strong suppression below TN2 indicates that a spin-gap opens in the excitation spectrum. High-resolution neutron inelastic scattering confirms that the magnetic dynamics are indeed gapped ({Delta}~5 meV) in the low-temperature magnetic phase, while simulations on the basis of the single-mode approximation suggest that Mn-spins residing on ad-jacent antiferromagnetic chains, establish sizable 2D correlations. Our analysis points that novel struc-tural degrees of freedom promote, cooperative magnetism and emerging dielectric properties in this non-perovskite-type of manganite.
The magnetic order and the spin dynamics in the antiferromagnetic entropy-stabilized oxide (Mg$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)O (MgO-ESO) have been studied using muon spin relaxation ($mu$SR) and inelastic neutron scattering. We find that antiferromagnetic order develops gradually in the sample volume as it is cooled below 140 K, becoming fully ordered around 100 K. The spin dynamics show a critical slowing down in the vicinity of the transition, and the magnetic order parameter grows continuously in the ordered state. These results indicate that the antiferromagnetic transition is continuous but proceeds with a Gaussian distribution of ordering temperatures. The magnetic contribution to the specific heat determined from inelastic neutron scattering likewise shows a broad feature centered around 120 K. High-resolution inelastic neutron scattering further reveals an initially gapped spectrum at low temperature which sees an increase in a quasielastic contribution upon heating until the ordering temperature.
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