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Effect of Coulomb interaction on the two-dimensional electronic structure of the van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$

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 Added by Masahiro Suzuki
 Publication date 2018
  fields Physics
and research's language is English




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In order to investigate the electronic properties of the semiconducting van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$ (CGT), where ferromagnetic layers are bonded through van der Waals forces, we have performed angle-resolved photoemission spectroscopy (ARPES) measurements and density-functional-theory (DFT+U) calculations. The valence-band maximum at the {Gamma} point is located $sim$ 0.2 eV below the Fermi level, consistent with the semiconducting property of CGT. Comparison of the experimental density of states with the DFT calculation has suggested that Coulomb interaction between the Cr 3d electrons U$_{rm eff}$ $sim$ 1.1 eV. The DFT+U calculation indicates that magnetic coupling between Cr atoms within the layer is ferromagnetic if Coulomb U $_{rm eff}$ is smaller than 3.0 eV and that the inter-layer coupling is ferromagnetic below U$_{rm eff}$ $sim$ 1.0 eV. We therefore conclude that, for U$_{rm eff}$ deduced by the experiment, the intra-layer Cr-Cr coupling is ferromagnetic and the inter-layer coupling is near the boundary between ferromagnetic and antiferromagnetic, which means experimentally deduced U$_{rm eff}$ is consistent with theoretical ferromagnetic condition.



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160 - M. Suzuki , B. Gao , G. Shibata 2021
The van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$ (CGT) has a two-dimensional crystal structure where each layer is stacked through van der Waals force. We have investigated the nature of the ferromagnetism and the weak perpendicular magnetic anisotropy (PMA) of CGT by means of X-ray absorption spectroscopy and X-ray magnetic circular dichroism (XMCD) studies of CGT single crystals. The XMCD spectra at the Cr $L_{2,3}$ edge for different magnetic field directions were analyzed on the basis of the cluster-model multiplet calculation. The Cr valence is confirmed to be 3+ and the orbital magnetic moment is found to be nearly quenched, as expected for the high-spin $t_{2g}$$^3$ configuration of the Cr$^{3+}$ ion. A large ($sim 0.2$ eV) trigonal crystal-field splitting of the $t_{2g}$ level caused by the distortion of the CrTe$_6$ octahedron has been revealed, while the single-ion anisotropy (SIA) of the Cr atom is found to have a sign {it opposite} to the observed PMA and too weak compared to the reported anisotropy energy. The present result suggests that anisotropic exchange coupling between the Cr atoms through the ligand Te $5p$ orbitals having strong spin-orbit coupling has to be invoked to explain the weak PMA of CGT, as in the case of the strong PMA of CrI$_3$.
We report the results of the pressure-dependent measurements of the static magnetization and of the ferromagnetic resonance (FMR) of Cr$_2$Ge$_2$Te$_6$ to address the properties of the ferromagnetic phase of this quasi-two-dimensional van der Waals magnet. The static magnetic data at hydrostatic pressures up to 3.4 GPa reveal a gradual suppression of ferromagnetism in terms of a reduction of the critical transition temperature, a broadening of the transition width and an increase of the field necessary to fully saturate the magnetization $M_{rm s}$. The value of $M_{rm s} simeq 3mu_{rm B}$/Cr remains constant within the error bars up to a pressure of 2.8 GPa. The anisotropy of the FMR signal continuously diminishes in the studied hydrostatic pressure range up to 2.39 GPa suggesting a reduction of the easy-axis type magnetocrystalline anisotropy energy (MAE). A quantitative analysis of the FMR data gives evidence that up to this pressure the MAE constant $K_{rm U}$, although getting significantly smaller, still remains finite and positive, i.e. of the easy-axis type. Therefore, a recently discussed possibility of switching the sign of the magnetocrystalline anisotropy in Cr$_2$Ge$_2$Te$_6$ could only be expected at still higher pressures, if possible at all due to the observed weakening of the ferromagnetism under pressure. This circumstance may be of relevance for the design of strain-engineered functional heterostructures containing layers of Cr$_2$Ge$_2$Te$_6$.
We study the magnetisation dynamics of a bulk single crystal Cr$_2$Ge$_2$Te$_6$ (CGT), by means of broadband ferromagnetic resonance (FMR), for temperatures from 60 K down to 2 K. We determine the Kittel relations of the fundamental FMR mode as a function of frequency and static magnetic field for the magnetocrystalline easy - and hard - axis. The uniaxial magnetocrystalline anisotropy constant is extracted and compared with the saturation magnetisation, when normalised with their low temperature values. The ratios show a clear temperature dependence when plotted in the logarithmic scale, which departs from the predicted Callen-Callen power law fit of a straight line, where the scaling exponent textit{n}, $K_{u}(T) propto [M_s(T)/M_s(2$ K$)]^n$, contradicts the expected value of 3 for uniaxial anisotropy. Additionally, the spectroscopic g-factor for both the magnetic easy - and hard - axis exhibits a temperature dependence, with an inversion between 20 K and 30 K, suggesting an influence by orbital angular momentum. Finally, we qualitatively discuss the observation of multi-domain resonance phenomena in the FMR spectras, at magnetic fields below the saturation magnetisation.
Anomalous Nernst effect, a result of charge current driven by temperature gradient, provides a probe of the topological nature of materials due to its sensitivity to the Berry curvature near the Fermi level. Fe3GeTe2, one important member of the recently discovered two-dimensional van der Waals magnetic materials, offers a unique platform for anomalous Nernst effect because of its metallic and topological nature. Here, we report the observation of large anomalous Nernst effect in Fe3GeTe2. The anomalous Hall angle and anomalous Nernst angle are about 0.07 and 0.09 respectively, far larger than those in common ferromagnets. By utilizing the Mott relation, these large angles indicate a large Berry curvature near the Fermi level, consistent with the recent proposal for Fe3GeTe2 as a topological nodal line semimetal candidate. Our work provides evidence of Fe3GeTe2 as a topological ferromagnet, and demonstrates the feasibility of using two-dimensional magnetic materials and their band topology for spin caloritronics applications.
Combining robust magnetism, strong spin-orbit coupling and unique thickness-dependent properties of van der Waals crystals could enable new spintronics applications. Here, using density functional theory, we propose the (MnSb$_2$Te$_4$)$cdot$(Sb$_2$Te$_3$)$_n$ family of stoichiometric van der Waals compounds that harbour multiple topologically-nontrivial magnetic phases. In the groundstate, the first three members of the family, i.e. MnSb$_2$Te$_4$, ($n=0$), MnSb$_4$Te$_7$, ($n=1$), and MnSb$_6$Te$_{10}$, ($n=2$), are 3D antiferromagnetic topological insulators (AFMTIs), while for $n geq 3$ a special phase is formed, in which a nontrivial topological order coexists with a partial magnetic disorder in the system of the decoupled 2D ferromagnets, whose magnetizations point randomly along the third direction. Furthermore, due to a weak interlayer exchange coupling, these materials can be field-driven into the FM Weyl semimetal ($n=0$) or FM axion insulator states ($n geq 1$). Finally, in two dimensions we reveal these systems to show intrinsic quantum anomalous Hall and AFM axion insulator states, as well as quantum Hall state, achieved under external magnetic field, but without Landau levels. Our results provide a solid computational proof that MnSb$_2$Te$_4$, is not topologically trivial as was previously believed that opens possibilities of realization of a wealth of topologically-nontrivial states in the (MnSb$_2$Te$_4$)$cdot$(Sb$_2$Te$_3$)$_n$ family.
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