A star-function based density functional study of the adsorption of Lennard-Jones fluid near its supercritical states

The goal of this paper is to show that the wetting behavior of simple fluids on a repulsive solid surface - especially the “drying” phenomenon - is closely related to the proximity of the supercritical state of the bulk fluids to their vapor-liquid coexistence region. We propose here a new DFT (the star-function based density functional theory, s-DFT) that is based on the functional Taylor expansion of the intrinsic free energy F[ρ] and the singlet direct correlation to arrive at closed-form expressions for both quantities without truncations or approximations. The two formulas are mutually consistent because of the introduction of a star function Sw that has been shown to be the functional primitive of the bridge function Bw, i.e. (L.L. Lee, J. Chem. Phys. 97 (1992) 8606 [34]). The new formulation is applied to the Lennard-Jones molecules adsorbed on a planar hard wall (LJ/HW). We carried out new Monte Carlo simulations for this system. Since the s-DFT uses a bridge function Bw, we demonstrate (i) the existence of a set of data (inverted from the MC information) that can perform as the bridge function and reproduce accurately the density profiles ; (ii) this set of data can be “fitted” by a function-form with acronym ZSEP; finally (iii) ZSEP expresses the bridge function Bw in terms of a new renormalized basis function γ_H, i.e. Bw(γH). The existence of a bridge function dispels some of the misconceptions that the bridge-function based formulations did not describe the “drying” behavior. We also show that for the high density case ZSEP equation can qualify as a “closure relation”, but seems to deteriorate for the two low-density supercritical states that are close to the bulk saturated liquid phase boundaries.     

Thermoelectric transport in graphene and 2D layered materials

ABSTRACT

In early 90s, Hicks and Dresselhaus proposed that low dimensional materials are advantages for thermoelectric applications due to the sharp features in their density-of-states, resulting in a high Seebeck coefficient and, potentially, in a high thermoelectric power factor. Two-dimensional (2D) materials are the latest class of low dimensional materials studied for thermoelectric applications. The experimental exfoliation of graphene, a single-layer of carbon atoms in 2004, triggered an avalanche of studies devoted to 2D materials in view of electronic, thermal, and optical applications. One can mix and match and stack 2D layers to form van der Waals hetero-structures. Such structures have extreme anisotropic transport properties. Both in-plane and cross-plane thermoelectric transport in these structures are of interest. In this short review article, we first review the progress achieved so far in the study of thermoelectric transport properties of graphene, the most widely studied 2D material, as a representative of interesting in-plane thermoelectric properties. Then, we turn our attention to the layered materials, in their cross-plane direction, highlighting their role as potential structures for solid-state thermionic power generators and coolers.     

Van der Waals coefficients and cohesive energies of lead chalcogenides

The cohesive energies of PbS PbSe and PbTe, having NaCl type of crystal structure, are calculated using the generalized Huggins-Mayer form (GHM) for the Born repulsion energy. The van der Waals interactions (VDW) are estimated from the London and Mayer formulae and compared with those estimated from the Slater-Kirkwood variational method. The cohesive energies calculated adopting the VDW coefficients calculated from the later method are in good agreement with the experimental values. The difference between the experimental cohesive energies and the calculated, assuming variational method, are 2·26, 2·97 and 3·75 eV respectively for PbS, PbSe and PbTe which are in good agreement with the reported values for the covalent bonding correction using Heitler-London-Lowdin method (HLL) which are respectively 2·1, 2·9 and 3·3 eV (Tanaka and Morita 1979).     

Monte Carlo Simulations of Binary Lennard–Jones Mixtures: A Test of the van der Waals One-Fluid Model

Monte Carlo simulations in the canonical ensemble have been performed in the liquid and supercritical regions of a binary Lennard–Jones mixture with differences in size parameters of 6.4% and energy parameters of 37%. The results are compared with a recent fundamental equation of state employing the van der Waals one-fluid model and new simulation data at the corresponding state conditions of the pure Lennard–Jones fluid. The van der Waals one-fluid model describes the mixture properties well at high densities, while at low densities the predicted internal energies and isochoric heat capacities are too low.     

Fully-Depleted PdTe2/WSe2 van der Waals Field Effect Transistor with High Light On/Off Ratio and Broadband Detection

Due to its unique band structure and topological properties, the 2D topological semimetal exhibits potential applications in photoelectric detection, polarization sensitive imaging, and Schottky barrier diodes. However, its inherent large dark current hinders the further improvement of the performance of the semimetal-based photodetectors. In this study, a van der Waals (vdWs) field effect transistor (FET) composed of semimetal PdTe₂ and transition metal dichalcogenides (TMDs) WSe₂ is fabricated, which exhibits high sensitivity photoelectric detection performance in a wide band from visible light (405 nm) to mid-infrared (5 µm). The dark current and the noise level in the device are greatly suppressed by the effective control of the gate. Benefiting from the extremely low dark current (1.2 pA), the device achieves an optical on/off ratio up to 10⁶, a high detectivity of 9.79 × 10¹³ Jones and a rapid response speed (219 and 45 µs). This research demonstrates the latent capacity of the 2D topological semimetal/TMDs vdWs FET for broadband, high-performance, and miniaturized photodetection.     

Interplay between Short‐ and Long‐Ranged Forces Leading to the Formation of Ag Nanoparticle Superlattice

Nanoparticle (NP) superlattices have attracted increasing attention due to their unique physicochemical properties. However, key questions persist regarding the correlation between short‐ and long‐range driving forces for nanoparticle assembly and resultant capability to predict the transient and final superlattice structure. Here the self‐assembly of Ag NPs in aqueous solutions is investigated by employing in situ liquid cell transmission electron microscopy, combined with atomic force microscopy‐based force measurements, and theoretical calculations. Despite the NPs exhibiting instantaneous Brownian motion, it is found that the dynamic behavior of NPs is correlated with the van der Waals force, sometimes unexpectedly over relatively large particle separations. After the NPs assemble into clusters, a delicate balance between the hydration and van der Waals forces results in a distinct distribution of particle separation, which is ascribed to layers of hydrated ions adsorbed on the NP surface. The study demonstrates pivotal roles of the complicated correlation between interparticle forces; potentially enabling the control of particle separation, which is critical for tailoring the properties of NP superlattices.     

PtTe2‐Based Type‐II Dirac Semimetal and Its van der Waals Heterostructure for Sensitive Room Temperature Terahertz Photodetection

Recent years have witnessed rapid progresses made in the photoelectric performance of two‐dimensional materials represented by graphene, black phosphorus, and transition metal dichalcogenides. Despite significant efforts, a photodetection technique capable for longer wavelength, higher working temperature as well as fast responsivity, is still facing huge challenges due to a lack of best among bandgap, dark current, and absorption ability. Exploring topological materials with nontrivial band transport leads to peculiar properties of quantized phenomena such as chiral anomaly, and magnetic‐optical effect, which enables a novel feasibility for an advanced optoelectronic device working at longer wavelength. In this work, the direct generation of photocurrent at low energy terahertz (THz) band at room temperature is implemented in a planar metal–PtTe₂–metal structure. The results show that the THz photodetector based on PtTe₂ with bow‐tie‐type planar contacts possesses a high photoresponsivity (1.6 A W^?1 without bias voltage) with a response time less than 20 µs, while the PtTe₂–graphene heterostructure‐based detector can reach responsivity above 1.4 kV W^?1 and a response time shorter than 9 µs. Remarkably, it is already exploitable for large area imaging applications. These results suggest that topological semimetals such as PtTe₂ can be ideal materials for implementation in a high‐performing photodetection system at THz band.     

Van der Waals Integration of Bismuth Quantum Dots–Decorated Tellurium Nanotubes (Te@Bi) Heterojunctions and Plasma‐Enhanced Optoelectronic Applications

Van der Waals (vdW)‐integrated heterojunctions have been widely investigated in optoelectronics due to their superior photoelectric conversion capability. In this work, 0D bismuth quantum dots (Bi QDs)‐decorated 1D tellurium nanotubes (Te NTs) vdW heterojunctions (Te@Bi vdWHs) are constructed by a facile bottom‐up assembly process. Transient absorption spectroscopy suggests that Te@Bi vdWH is a promising candidate for new‐generation optoelectronic devices with fast response properties. The subsequent experiments and density functional theory calculations demonstrate the vdW interaction between Te NTs and Bi QDs, as well as the enhanced optoelectronic characteristics owing to the plasma effects at the interface between Te NTs and Bi QDs. Moreover, Te@Bi vdWHs‐based photodetectors show significantly improved photoresponse behavior in the ultraviolet region compared to pristine Te NTs or Bi QDs‐based photodetectors. The proposed integration of vdWHs is expected to pave the way for constructing new nanoscale heterodevices.     

A size-dependent model for instability analysis of paddle-type and double-sided NEMS measurement sensors in the presence of centrifugal force

Paddle-type and double-sided nanostructures have much potential for measuring the angular speed in rotary systems and aerospace applications. While most investigations in the literature have concentrated on the electromechanical performance of conventional beam-type nanostructures, few researchers have addressed the performance of these systems. The pull-in instability of the cantilever paddle-type and double-sided sensors in the presence of the centrifugal force have been investigated. The nonlinear governing equations are solved and the obtained results are compared with the numerical solution. The influences of the van der Waals force, geometric parameters, angular speed, and size phenomenon on the instability performance have been demonstrated.     

A three‐dimensional surface stress tensor formulation for simulation of adhesive contact in finite deformation

A three‐dimensional surface adhesive contact formulation is proposed to simulate macroscale adhesive contact interaction characterized by the van der Waals interaction between arbitrarily shaped deformable continua under finite deformation. The proposed adhesive contact formulation uses a double‐layer surface integral to replace the conventional double volume integration to compute the adhesive contact force vector. Considering nonlinear finite deformation, we have derived the surface stress tensor and the corresponding tangent stiffness matrix in a Galerkin weak formulation. With the surface stress formulation, the adhesive contact problems are solved in the framework of nonlinear continuum mechanics by using the standard Lagrange finite element method. Surface stress tensors are formulated for both interacting bodies. Numerical examples show that the proposed surface contact algorithm is accurate, efficient, and reliable for three‐dimensional adhesive contact problems of large deformations for both quasi‐static and dynamic simulations. Copyright © 2015 John Wiley & Sons, Ltd.