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تسجيل مستخدم جديدElectronic structure of the kagome staircase compounds Ni3V2O8 and Co3V2O8
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The electronic structure of the kagome staircase compounds, Ni3V2O8 and Co3V2O8, has been investigated using soft x-ray absorption, soft x-ray emission, and resonant inelastic x-ray scattering (RIXS). Comparison between the two compounds, and with first principles band structure calculations and crystal-field multiplet models, provide unique insight into the electronic structure of the two materials. Whereas the location of the narrow (Ni,Co) d bands is predicted to be close to EF, we experimentally find they lie deeper in the occupied O 2p and unoccupied V 3d manifolds, and determine their energy via measured charge-transfer excitations. Additionally, we find evidence for a dd excitation at 1.5 eV in Ni3V2O8, suggesting the V d states may be weakly occupied in this compound, contrary to Co3V2O8. Good agreement is found between the crystal-field dd excitations observed in the experiment and predicted by atomic multiplet theory.
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At zero magnetic field, a series of five phase transitions occur in Co3V2O8. The Neel temperature, TN=11.4 K, is followed by four additional phase changes at T1=8.9 K, T2=7.0 K, T3=6.9 K, and T4=6.2 K. The different phases are distinguished by the co
mmensurability of the b-component of its spin density wave vector. We investigate the stability of these various phases under magnetic fields through dielectric constant and magnetic susceptibility anomalies. The field-temperature phase diagram of Co3V2O8 is completely resolved. The complexity of the phase diagram results from the competition of different magnetic states with almost equal ground state energies due to competing exchange interactions and frustration.
Co3V2O8 (CVO) has a geometrically frustrated magnetic lattice, a Kagome staircase. The crystal structure consists of two inequivalent Co sites, one-dimensional chains of Co(2) spine sites, linked by Co(1) cross-tie sites. Neutron powder diffraction h
as been used to solve the basic magnetic and crystal structures of this system, while polarized and unpolarized single crystal diffraction measurements have been used to reveal a variety of incommensurate phases, interspersed with lock-in transitions to commensurate phases. CVO initially orders magnetically at 11.3 K into an incommensurate, transversely polarized, spin density wave state, with wave vector k=(0,delta,0) with delta=0.55 and the spin direction along the a axis. Delta is found to decrease monotonically with decreasing temperature, and then it locks into a commensurate antiferromagnetic structure with delta=0.5 for 6.9<T<8.6 K. Below 6.9 K the magnetic structure becomes incommensurate again. Delta continues to decrease with decreasing temperature, and locks-in again at delta=1/3 over a narrow temperature range (6.2<T<6.5 K). The system then undergoes a strongly first order transition to the ferromagnetic ground state (delta=0) at Tc=6.2 K. A dielectric anomaly is observed around the ferromagnetic transition temperature of 6.2 K, demonstrating a significant spin-charge coupling present in CVO. A theory based on group theory analysis and a minimal Ising model with competing exchange interactions can explain the basic features of the magnetic ordering.
We present powder and single-crystal neutron diffraction and bulk measurements of the Kagome-staircase compound Ni3V2O8 (NVO) in fields up to 8.5T applied along the c-direction. (The Kagome plane is the a-c plane.) This system contains two types of N
i ions, which we call spine and cross-tie. Our neutron measurements can be described with the paramagnetic space group Cmca for T < 15K and each observed magnetically ordered phase is characterized by the appropriate irreducible representation(s). Our zero-field measurements show that at T_PH=9.1K NVO undergoes a transition to an incommensurate order which is dominated by a longitudinally-modulated structure with the spine spins mainly parallel to the a-axis. Upon further cooling, a transition is induced at T_HL=6.3K to an elliptically polarized incommensurate structure with both spine and cross-tie moments in the a-b plane. At T_LC=4K the system undergoes a first-order phase transition, below which the magnetic structure is a commensurate antiferromagnet with the staggered magnetization primarily along the a-axis and a weak ferromagnetic moment along the c-axis. A specific heat peak at T_CC=2.3K indicates an additional transition, which we were however not able to relate to a change of the magnetic structure. Neutron, specific heat, and magnetization measurements produce a comprehensive temperature-field phase diagram. The symmetries of the two incommensurate magnetic phases are consistent with the observation that only one phase has a spontaneous ferroelectric polarization. All the observed magnetic structures are explained theoretically using a simplified model Hamiltonian, involving competing nearest- and next-nearest-neighbor exchange interactions, spin anisotropy, Dzyaloshinskii-Moriya and pseudo-dipolar interactions.
The magnetic properties of Co3V2O8 have been studied by single-crystal neutron-diffraction. In zero magnetic field, the observed broadening of the magnetic Bragg peaks suggests the presence of disorder both in the low-temperature ferromagnetic and in
the higher-temperature antiferromagnetic state. The field dependence of the intensity and position of the magnetic reflections in Co3V2O8 reveals a complex sequence of phase transitions in this Kagome staircase compound. For H//a, a commensurate-incommensurate-commensurate transition is found in a field of 0.072 T in the antiferromagnetic phase at 7.5 K. For H//c at low-temperature, an applied field induces an unusual transformation from a ferromagnetic to an antiferromagnetic state at about 1 T accompanied by a sharp increase in magnetisation.
The dielectric constant of the Kagome staircase-like Co3V2O8 polycrystalline compound has been measured as function of temperature and magnetic field up to 14T. It is found that the application of an external magnetic field suppresses the anomaly for
the dielectric constant beyond 6.1K. Furthermore, its magnetic field dependence reveals a negative magnetocapacitance which is proportional to the magnetic susceptibility, suggesting a common magnetostrictive origin for the magnetic field dependence of the two quantities. This result is very different from that obtained from the isostructural compound Ni3V2O8 that presents a peak in the dielectric constant at the incommensurate magnetic phase transition coupled to a sign change of the magnetocapacitance.
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