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We report results of investigation of the phonon and thermal properties of the exfoliated films of layered single crystals of antiferromagnetic FePS3 and MnPS3 semiconductors. The Raman spectroscopy was conducted using three different excitation lasers with the wavelengths of 325 nm (UV), 488 nm (blue), and 633 nm (red). The resonant UV-Raman spectroscopy reveals new spectral features, which are not detectable via visible Raman light scattering. The thermal conductivity of FePS3 and MnPS3 thin films was measured by two different techniques: the steady-state Raman optothermal and transient time-resolved magneto-optical Kerr effect. The Raman optothermal measurements provided the orientation-average thermal conductivity of FePS3 to be 1.35 W/mK at room temperature. The transient measurements revealed that the through-plane and in-plane thermal conductivity of FePS3 is 0.85 W/mK and 2.7 W/mK, respectively. The films of MnPS3 have higher thermal conductivity of 1.1 W/mK through-plane and 6.3 W/mK in-plane. The data obtained by both techniques reveal strong thermal anisotropy of the films and the dominant contribution of phonons to heat conduction. Our results are important for the proposed applications of the antiferromagnetic semiconductor thin films in spintronic devices.
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Recently it was discovered that van der Waals-bonded magnetic materials retain long range magnetic ordering down to a single layer, opening many avenues in fundamental physics and potential applications of these fascinating materials. One such material is FePS3, a large spin (S=2) Mott insulator where the Fe atoms form a honeycomb lattice. In the bulk, FePS3 has been shown to be a quasi-two-dimensional-Ising antiferromagnet, with additional features in the Raman spectra emerging below the Neel temperature of approximately 120 K. Using magneto-Raman spectroscopy as an optical probe of magnetic structure, we show that one of these Raman-active modes in the magnetically ordered state is actually a magnon with a frequency of of approximately 3.7 THz (122 cm-1). Contrary to previous work, which interpreted this feature as a phonon, our Raman data shows the expected frequency shifting and splitting of the magnon as a function of temperature and magnetic field, respectively, where we determine the g-factor to be approximately 2. In addition, the symmetry behavior of the magnon is studied by polarization-dependent Raman spectroscopy and explained using the magnetic point group of FePS3.
Van der Waals heterostructure based on layered two-dimensional (2D) materials offers unprecedented opportunities to create materials with atomic precision by design. By combining superior properties of each component, such heterostructure also provides possible solutions to address various challenges of the electronic devices, especially those with vertical multilayered structures. Here, we report the realization of robust memristors for the first time based on van der Waals heterostructure of fully layered 2D materials (graphene/MoS2-xOx/graphene) and demonstrate a good thermal stability lacking in traditional memristors. Such devices have shown excellent switching performance with endurance up to 107 and a record-high operating temperature up to 340oC. By combining in situ high-resolution TEM and STEM studies, we have shown that the MoS2-xOx switching layer, together with the graphene electrodes and their atomically sharp interfaces, are responsible for the observed thermal stability at elevated temperatures. A well-defined conduction channel and a switching mechanism based on the migration of oxygen ions were also revealed. In addition, the fully layered 2D materials offer a good mechanical flexibility for flexible electronic applications, manifested by our experimental demonstration of a good endurance against over 1000 bending cycles. Our results showcase a general and encouraging pathway toward engineering desired device properties by using 2D van der Waals heterostructures.
The high breakdown current densities and resilience to scaling of the metallic transition metal trichalcogenides TaSe3 and ZrTe3 make them of interest for possible interconnect applications, and it motivates this study of their thermal conductivities and phonon properties. These crystals consist of planes of strongly bonded one-dimensional chains more weakly bonded to neighboring chains. Phonon dispersions and the thermal conductivity tensors are calculated using density functional theory combined with an iterative solution of the phonon Boltzmann transport equation. The phonon velocities and the thermal conductivities of TaSe3 are considerably more anisotropic than those of ZrTe3. The maximum LA velocity in ZrTe3 occurs in the cross-chain direction, and this is consistent with the strong cross-chain bonding that gives rise to large Fermi velocities in that direction. The thermal conductivities are similar to those of other metallic two-dimensional transition metal dichalcogenides. At room temperature, a significant portion of the heat is carried by the optical modes. In the low frequency range, the phonon lifetimes and mean free paths in TaSe3 are considerably shorter than those in ZrTe3. The shorter lifetimes in TaSe3 are consistent with the presence of lower frequency optical branches and zone-folding features in the acoustic branches that arise due to the doubling of the TaSe3 unit cell within the plane.
Precise manipulation of electronic band structures of two-dimensional (2D) transition metal dichalcogenides and oxides (TMD&Os) via localised strain engineering is an exciting avenue for exploiting their unique characteristics for electronics, optoelectronics, and nanoelectromechanical systems (NEMS) applications. This work experimentally demonstrates that mechanically-induced electrical transitions can be engineered in quasi-2D molybdenum disulphide (MoS2) and molybdenum trioxide (MoO3) using an in situ electrical nanoindentation technique. It is shown that localised strains on such quasi-2D layers can induce carrier transport alterations, thereby changing their electrical conduction behaviour. Such strain effects offer a potential tool for precisely manipulating the electronic transport properties of 2D TMD&Os, and understanding the interactions of the atomic electronic states in such layered materials.
Thermal transport in solids changes its nature from phonon propagation that suffers from perturbative scattering to thermally activated hops between localized vibrational modes as the level of disorder increases. Models have been proposed to understand these two distinct extremes that predict opposite temperature dependence of the thermal conductivity, but not for the transition or the intermediate regime. Here we explore thermal transport in two-dimensional crystalline and amorphous silica with varying levels of disorder, {alpha}, by performing atomistic simulations as well as analysis based on the kinetic and Allen-Feldman theories. We demonstrate the crossover between the crystalline and amorphous regimes at {alpha} ~ 0.3, which can be identified by a turnover of the temperature dependence in thermal conductivity, and explained by the dominance of thermal hopping processes. The determination of this critical disorder level is also validated by the analysis of the participation ratio of localized vibrational modes, and the spatial localization of heat flux. These factors can serve as key indicators in characterizing the transition in heat transport mechanisms.
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