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Nanomechanical probing and strain tuning of the Curie temperature in suspended Cr$_2$Ge$_2$Te$_6$ heterostructures

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 Publication date 2021
  fields Physics
and research's language is English




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Two-dimensional (2D) magnetic materials with strong magnetostriction, like Cr$_2$Ge$_2$Te$_6$ (CGT), provide opportunities for tuning their magnetic state with potential applications in spintronic and magneto-mechanical devices. However, realizing this potential requires understanding their mechanical properties, such as the Youngs modulus, and the ability to controllably strain the magnets and monitor their ferromagnetic Curie temperature $T_{rm C}$ on a device level. In this work, we suspend thin CGT layers to form nanomechanical membrane resonators. We then probe the mechanical and magnetic properties of CGT as a function of temperature and strain by static and dynamic nanomechanical methods. Pronounced signatures of magneto-elastic coupling are observed in the temperature-dependent resonance frequency of these membranes at the $T_{rm C}$. We further utilize CGT in heterostructures with thin WSe$_2$ and FePS$_3$ layers to control the strain in CGT flakes and quantitatively probe the transition temperatures of all materials involved. In addition, an enhancement of $T_{rm C}$ by $2.5pm0.6$ K in CGT is realized by electrostatic force straining the heterostructure of $0.016%$ in the absence of an external magnetic field. Nanomechanical strain thus offers a compelling degree of freedom to probe and control magnetic phase transitions in 2D layered ferromagnets and heterostructures.



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Electrical control of magnetism of a ferromagnetic semiconductor offers exciting prospects for future spintronic devices for processing and storing information. Here, we report observation of electrically modulated magnetic phase transition and magnetic anisotropy in thin crystal of Cr$_2$Ge$_2$Te$_6$ (CGT), a layered ferromagnetic semiconductor. We show that heavily electron-doped ($sim$ $10^{14}$ cm$^{-2}$) CGT in an electric double-layer transistor device is found to exhibit hysteresis in magnetoresistance (MR), a clear signature of ferromagnetism, at temperatures up to above 200 K, which is significantly higher than the known Curie temperature of 61 K for an undoped material. Additionally, angle-dependent MR measurements reveal that the magnetic easy axis of this new ground state lies within the layer plane in stark contrast to the case of undoped CGT, whose easy axis points in the out-of-plane direction. We propose that significant doping promotes double-exchange mechanism mediated by free carriers, prevailing over the superexchange mechanism in the insulating state. Our findings highlight that electrostatic gating of this class of materials allows not only charge flow switching but also magnetic phase switching, evidencing their potential for spintronics applications.
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.
Graphene sandwiched between semiconducting monolayers of ferromagnet Cr$_2$Ge$_2$Te$_6$ and transition-metal dichalcogenide WS$_2$ acquires both spin-orbit (SO), of valley-Zeeman and Rashba types, and exchange couplings. Using first-principles combined with quantum transport calculations, we predict that such doubly proximitized graphene within van der Waals heterostructure will exhibit SO torque driven by unpolarized charge current. This system lacking spin Hall current, putatively considered to be necessary for efficient damping-like (DL) SO torque that plays a key role in magnetization switching, demonstrates how DL torque component can be generated solely by skew-scattering off spin-independent potential barrier or impurities in purely two-dimensional electronic transport due to the presence of proximity SO coupling and its spin texture tilted out-of-plane. This leads to current-driven nonequilibrium spin density emerging in all spatial directions, whose cross product with proximity magnetization yields DL SO torque, unlike the ballistic regime with no scatterers in which only field-like (FL) SO torque appears. In contrast to SO torque on conventional metallic ferromagnets in contact with three dimensional SO-coupled materials, the ratio of FL and DL torque can be tuned by more than an order of magnitude via combined top and back gates.
Full experimental control of local spin-charge interconversion is of primary interest for spintronics. Heterostructures combining graphene with a strongly spin-orbit coupled two-dimensional (2D) material enable such functionality by design. Electric spin valve experiments have provided so far global information on such devices, while leaving the local interplay between symmetry breaking, charge flow across the heterointerface and aspects of topology unexplored. Here, we utilize magneto-optical Kerr microscopy to resolve the gate-tunable, local current-induced spin polarisation in graphene/WTe$_2$ van der Waals (vdW) heterostructures. It turns out that even for a nominal in-plane transport, substantial out-of-plane spin accumulation is induced by a corresponding out-of-plane current flow. We develop a theoretical model which explains the gate- and bias-dependent onset and spatial distribution of the massive Kerr signal on the basis of interlayer tunnelling, along with the reduced point group symmetry and inherent Berry curvature of the heterostructure. Our findings unravel the potential of 2D heterostructure engineering for harnessing topological phenomena for spintronics, and constitute an important further step toward electrical spin control on the nanoscale.
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$_3$.
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