We investigate picosecond spin-currents across Au/iron-garnet interfaces in response to ultrafast laser heating of the electrons in the Au film. In the picoseconds after optical heating, interfacial spin currents occur due to an interfacial temperature difference between electrons in the metal and magnons in the insulator. We report measurements of this interfacial longitudinal spin Seebeck effect between Au and rare-earth iron-garnet insulators, i.e. RE3Fe5O12, where RE is Y, Eu, Tb, Tm. We use time domain thermoreflectance (TDTR) measurements to characterize the thermal response of the bilayer to ultrafast optical heating. We use timeresolved magneto-optic Kerr effect (TR-MOKE) measurements of the Au layer to measure the time-evolution of spin accumulation in the Au film. We observe a spin Seebeck effect between Au/TmIG that is three times larger than for an Au/YIG bilayer. The interfacial thermal
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. Raman spectroscopy was conducted using three different excitation lasers with wavelengths of 325 nm (UV), 488 nm (blue), and 633 nm (red). UV-Raman spectroscopy reveals 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 ± 0.32 W m-1 K-1 at room temperature. The transient measurements revealed that the through-plane and in-plane thermal conductivity of FePS3 are 0.85 ± 0.15 and 2.7 ± 0.3 W m-1 K-1, respectively. The films of MnPS3 have higher thermal conductivity of 1.1 ± 0.2 W m-1 K-1 through-plane and 6.3 ± 1.7 W m-1 K-1 in-plane. The data obtained by the two techniques are in agreement and reveal strong thermal anisotropy of the films and the dominance of phonon contribution to heat conduction. The obtained results are important for the interpretation of electric switching experiments with antiferromagnetic materials as well as for the proposed applications of the antiferromagnetic semiconductors in spintronic devices.
We describe an optical pump/probe system for sensitive measurements of time-resolved optical measurements of material dynamics. The instrument design is optimized for time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of dynamics in magnetic materials. The system also allows for time-domain thermoreflectance (TDTR) measurements of thermal transport properties and picosecond acoustic measurements of film thickness and/or elastic constants. The system has several advantages over the conventional designs for TR-MOKE and/or TDTR systems. Measurements of pump-induced changes to the probe beam intensity are shot-noise limited. The system's design allows for MOKE and/or thermoreflectance measurements of both sides of a sample. Pumping and probing the sample on opposite sides allows nanoscale flash diffusivity measurements of transport properties. The wavelengths of the pump and probe beams are straightforward to tune between 350-525 nm and 690-1050 nm. A tunable wavelength allows for optical resonances in a wide array of materials to be excited and/or probed. Finally, the setup is calibrated to allow for the real and imaginary components of Kerr signals to be separately quantified.
Wafer-scale MoS2 growth at arbitrary integer layer number is demonstrated by a technique based on the decomposition of carbon disulfide on a hot molybdenum filament, which yields volatile MoS x precursors that precipitate onto a heated wafer substrate. Colorimetric control of the growth process allows precise targeting of any integer layer number. The method is inherently free of particulate contamination, uses inexpensive reactants without the pyrophoricity common to metal-organic precursors, and does not rely on particular gas-flow profiles. Raman mapping and photoluminescence mapping, as well as imaging by electron microscopy, confirm the layer homogeneity and crystalline quality of the resultant material. Electrical characterization revealed microampere output current, outstanding device-to-device consistency, and exceptionally low noise level unparalleled even by the exfoliated material, while other transport properties are obscured by high-resistance contacts typical to MoS2 devices.
Transition metal dichalcogenides (TMDs) are exciting new materials that have received much attention due to their semiconducting properties in the direct bandgap. Well-studied TMDs, such as molybdenum disulfide (MoS 2 ) and tungsten diselenide (WSe 2 ), exhibit a direct bandgap in the monolayer form, but an indirect bandgap in the bulk form. Rhenium disulfide (ReS 2 ), on the other hand, is a new TMD that is unique in its ability to retain a direct bandgap independent of thickness. By using chemical vapor deposition (CVD), few-layer ReS 2 is synthesized and characterized by optical methods such as Raman spectroscopy and photoluminescence. We also show characterization results for atomic force microscopy (AFM), x-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM), transmission electron microscope (TEM), and electrical transport to determine thickness, crystallinity, homogeneity, and electrical characteristics for use in future flexible electronics.
Ultrafast control of magnetic order in materials requires a fundamental understanding of how energy and angular momentum flow between electronic, magnetic, and vibrational degrees-of-freedom. We investigate the ultrafast response of Au/TmIG and Au/YIG bilayers to ultrafast laser heating of the Au electrons. In the picoseconds after heating, large interfacial spin currents occur due to a temperature imbalance between electrons and phonons in the metal, and magnons and phonons in the magnetic insulator. We utilize four different optical probes to develop a complete picture of the heat and spin transport in Au/TmIG and Au/YIG. Magneto-optic Kerr effect measurements of Au at a wavelength of 800 nm detects the spin accumulation in the normal metal that results from interfacial spin-currents. Magneto-optic Kerr effect measurements at 400 nm monitor the ultrafast magnetization dynamics of the garnet insulator that occur due to increases in magnon population. Finally, thermoreflectance measurements at 690 and 950 nm monitor the temperature evolution of the Au electrons and phonons, respectively. Together, these measurements allow us to estimate the magnitude of the transport coefficients responsible for the longitudinal spin-Seebeck effect in these systems. These coefficients include the electron-magnon conductance of the Au/TmIG and Au/YIG interfaces, the electron-phonon coupling in the Au layer, and the magnon-phonon coupling in the TmIG and YIG layers.
Gold islands are typically associated with high binding affinity to adsorbates and catalytic activity. Here we present the growth of dispersed nanoscale gold islands on single layer MoS2, prepared on an inert SiO2/Si support by chemical vapor deposition. This study offers a combination of growth process development, optical characterization, photoelectron spectroscopy at submicron spatial resolution, and advanced density functional theory modeling for detailed insight into the electronic interaction between gold and single-layer MoS2. In particular, we find the gold density of states in Au/MoS2/SiO2/Si to be far less well-defined than Au islands on other 2-dimensional materials such as graphene, for which we also provide data. We attribute this effect to the presence of heterogeneous Au adatom/MoS2-support interactions within the nanometer-scale gold cluster. Theory predicts that CO will exhibit adsorption energies in excess of 1 eV at the Au cluster edges, where the local density of states is dominated by Au 5d(z)2 symmetry.
Chemical vapor deposition allows the preparation of few-layer films of MoTe2 in three distinct structural phases depending on the growth quench temperature: 2H, 1T', and 1T. We present experimental and computed Raman spectra for each of the phases and utilize transport measurements to explore the properties of the 1T MoTe2 phase. Density functional theory modeling predicts a (semi-)metallic character. Our experimental 1T films affirm the former, show facile μA-scale source-drain currents, and increase in conductivity with temperature, different from the 1T' phase. Variation of the growth method allows the formation of hybrid films of mixed phases that exhibit susceptibility to gating and significantly increased conductivity.
Growth by chemical vapor deposition (CVD) leads to multilayer WS2 of very high quality, based on high-resolution angle-resolved photoemission spectroscopy. The experimental valence band electronic structure is considered to be in good agreement with that obtained from density functional theory calculations. We find the spin-orbit splitting at the K¯ point to be 420 ± 20 meV with a hole effective mass of −0.35 ± 0.02 me for the upper spin-orbit component (the branch closer to the Fermi level) and −0.43 ± 0.07 me for the lower spin-orbit component. As predicted by theory, a thickness-dependent increase of bandwidth is observed at the top of the valence band, in the region of the Brillouin zone center. The top of the valence band of the CVD-prepared films exhibits a substantial binding energy, consistent with n-type behavior, and in agreement with transistor characteristics acquired using devices incorporating the same WS2 material.
We demonstrate bandgap tuning of a single-layer MoS2 film on SiO2/Si via substitution of its sulfur atoms by selenium through a process of gentle sputtering, exposure to a selenium precursor, and annealing. We characterize the substitution process both for S/S and S/Se replacement. Photoluminescence and, in the latter case, X-ray photoelectron spectroscopy provide direct evidence of optical band gap shift and selenium incorporation, respectively. We discuss our experimental observations, including the limit of the achievable bandgap shift, in terms of the role of stress in the film as elucidated by computational studies, based on density functional theory. The resultant films are stable in vacuum, but deteriorate under optical excitation in air.