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Register a new userEquipartition of Energy Defines the Size-Thickness Relationship in Liquid-Exfoliated Nanosheets
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Liquid phase exfoliation is a commonly used method to produce 2D nanosheets from a range of layered crystals. However, such nanosheets display broad size and thickness distributions and correlations between area and thickness, issues that limit nanosheet application potential. To understand the factors controlling the exfoliation process, we have liquid-exfoliated 11 different layered materials, size-selecting each into fractions before using AFM to measure the nanosheet length, width, and thickness distributions for each fraction. The resultant data show a clear power-law scaling of nanosheet area with thickness for each material. We have developed a simple nonequilibrium thermodynamics-based model predicting that the power-law prefactor is proportional to both the ratios of in-plane-tearing/out-of-plane-peeling energies and in-plane/out-of-plane moduli. By comparing the experimental data with the modulus ratio calculated from first-principles, we find close agreement between experiment and theory. This supports our hypothesis that energy equipartition holds between nanosheet tearing and peeling during sonication-assisted exfoliation.
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For many 2D materials, optical and Raman spectra are richly structured, and convey information on a range of parameters including nanosheet size and defect content. By contrast, the equivalent spectra for h-BN are relatively simple, with both the absorption and Raman spectra consisting of a single feature each, disclosing relatively little information. Here, the ability to size-select liquid-exfoliated h-BN nanosheets has allowed us to comprehensively study the dependence of h-BN optical spectra on nanosheet dimensions. We find the optical extinction coefficient spectrum to vary systematically with nanosheet lateral size due to the presence of light scattering. Conversely, once light scattering has been decoupled to give the optical absorbance spectra, we find the size dependence to be mostly removed save for a weak but well-defined variation in energy of peak absorbance with nanosheet thickness. This finding is corroborated by our ab initio GW and Bethe-Salpeter equation calculations, which include electron correlations and quasiparticle self-consistency (QSGW). In addition, while we find the position of the sole h-BN Raman line to be invariant with nanosheet dimensions, the linewidth appears to vary weakly with nanosheet thickness. These size-dependent spectroscopic properties can be used as metrics to estimate nanosheet thickness from spectroscopic data.
We studied the stability and superconductivity of FeSe nanosheets during an in-air device fabrication process. Methods were developed to improve the exfoliation yield and to maintain the superconductivity of FeSe. Raman spectroscopy, atomic force microscopy, optical microscopy and time-of-flight-secondary-ion-mass-spectroscopy measurements show that FeSe nanosheets decayed in air. Precipitation of Se particles and iron oxidation likely occurred during the decay process. Transport measurements revealed that the superconductivity of FeSe disappeared during a conventional electron beam lithography process. Shadow mask evaporation and transfer onto pre-defined electrodes methods were shown to be effective in maintaining the superconductivity after the in-air device fabrication process. These methods developed provide a way of making high quality FeSe nano-devices.
We report piezoelectric response in liquid phase exfoliated MoS2 nanosheets with desired structure and morphology. The piezoelectric effect in liquid phase exfoliated few layers of MoS2 flakes is interesting as it may allow the scalable fabrication of electronic devices such as self-powered electronics, piezoelectric transformers, antennas and more. The piezo force microscopy (PFM) measurements were used to quantify the amplitude and phase loop, which shows strong piezoelectric coefficient. Herein, the piezoelectric response in few layers of MoS2 is attributed to the defects formed in it during the synthesis procedure. The presence of defects is confirmed by XPS analysis
The turbulence of superfluid helium is investigated numerically at finite temperature. Direct numerical simulations are performed with a truncated HVBK model, which combines the continuous description of the Hall-Vinen-Bekeravich-Khalatnikov equations with the additional constraint that this continuous description cannot extend beyond a quantum length scale associated with the mean spacing between individual superfluid vortices. A good agreement is found with experimental measurements of the vortex density. Besides, by varying the turbulence intensity only, it is observed that the inter-vortex spacing varies with the Reynolds number as $Re^{-3/4}$, like the viscous length scale in classical turbulence. In the high temperature limit, Kolmogorovs inertial cascade is recovered, as expected from previous numerical and experimental studies. As the temperature decreases, the inertial cascade remains present at large scales while, at small scales, the system evolves towards a statistical equipartition of kinetic energy among spectral modes, with a characteristic $k^2$ velocity spectrum. The accumulation of superfluid excitations on a range of mesoscales enables the superfluid to keep dissipating kinetic energy through mutual friction with the residual normal fluid, although the later becomes rare at low temperature. It is found that most of the superfluid vorticity can concentrate on these mesoscales at low temperature, while it is concentrated in the inertial range at higher temperature. This observation should have consequences on the interpretation of decaying turbulence experiments, which are often based on vortex line density measurements.
Many atomic liquids can form transient covalent bonds reminiscent of those in the corresponding solid states. These directional interactions dictate many important properties of the liquid state, necessitating a quantitative, atomic-scale understanding of bonding in these complex systems. A prototypical example is liquid silicon, wherein transient covalent bonds give rise to local tetrahedral order and consequent non-trivial effects on liquid state thermodynamics and dynamics. To further understand covalent bonding in liquid silicon, and similar liquids, we present an ab initio simulation-based approach for quantifying the structure and dynamics of covalent bonds in condensed phases. Through the examination of structural correlations among silicon nuclei and maximally localized Wannier function centers, we develop a geometric criterion for covalent bonds in liquid Si. We use this to monitor the dynamics of transient covalent bonding in the liquid state and estimate a covalent bond lifetime. We compare covalent bond dynamics to other processes in liquid Si and similar liquids and suggest experiments to measure the covalent bond lifetime.
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