Frustrated van der Waals heterostructures.

Geometrical frustration results from the packing of constituents in a lattice, where the constituents have conflicting forces. The phenomenon is known in glass materials, and this work expands the concept of geometrical frustration into the realm of van der Waals two-dimensional materials. Using density functional theory with the rSCAN + rVV10 exchange-correlation potential, we find a number of two-dimensional heterostructures with alternating strains, where one layer is strained and the adjacent layer is compressed.

A case study using spectroscopy and computational modelling for Co speciation in a deep eutectic solvent.

Cobalt has a vital role in the manufacturing of reliable and sustainable clean energy technologies. However, the forecasted supply deficit for cobalt is likely to reach values of 150 kT by 2030. Therefore, it is paramount to consider end-of-life devices as secondary resources for cobalt.

Broken-gap energy alignment in two-dimensional van der Waals heterostructures for multifunctional tunnel diodes.

Two-dimensional (2D) materials are promising platforms for future nanoelectronic technologies as they provide the building blocks for atomically thin devices, including switches, amplifiers, and oscillators. When 2D materials are layered on top of each other, forming van der Waals heterostructures (vdWHs), they can provide unique properties not possessed by the individual layers. Here we consider the vdWHs HfS/MoTe, HfS/WTe, 1T-HfS/WTe, TiS/WSe, TiS/ZnO, and TiSe/WTe as potential Esaki (or tunnel) diodes that can be incorporated into electronic devices.

Blocking Directional Lithium Diffusion in Solid-State Electrolytes at the Interface: First-Principles Insights into the Impact of the Space Charge Layer.

Understanding the degradation mechanisms in solid-state lithium-ion batteries at interfaces is fundamental for improving battery performance and for designing recycling methodologies for batteries. A key source of battery degradation is the presence of the space charge layer at the solid-state electrolyte-electrode interface and the impact that this layer has on the thermodynamics of the electrolyte structure. Currently, LiGePS in its pristine form has one of the highest lithium conductivities and has been used as a template for designing even higher conductivity derived structures.

Naturally-meaningful and efficient descriptors: machine learning of material properties based on robust one-shot ab initio descriptors.

Establishing a data-driven pipeline for the discovery of novel materials requires the engineering of material features that can be feasibly calculated and can be applied to predict a material's target properties. Here we propose a new class of descriptors for describing crystal structures, which we term Robust One-Shot Ab initio (ROSA) descriptors. ROSA is computationally cheap and is shown to accurately predict a range of material properties.

Ferroelectric van der Waals heterostructures of CuInPSfor non-volatile memory device applications.

Two-dimensional (2D) ferroelectric materials are providing promising platforms for creating future nano- and opto-electronics. Here we propose new hybrid van der Waals heterostructures, in which the 2D ferroelectric material CuInPS(CIPS) is layered on a 2D semiconductor for near-infrared (NIR) memory device applications. Using density functional theory, we show that the band gap of the hybrid bilayers formed with CIPS can be tuned and that the optical and electronic properties can be successfully modulated via ferroelectric switching.

Improving sensing of formaldehyde using ZnO nanostructures with surface-adsorbed oxygen.

Detection of pollutant gases, such as formaldehyde (HCHO), in our homes and surrounding environment is of high importance for our health and safety. The effect of surface defects and specifically pre-adsorbed oxygen on the gas sensing reaction of HCHO with ZnO nanostructures is largely unknown. Using density functional theory, nonequilibrium Green's function method and molecular dynamics (AIMD) simulations, we show that the presence of surface oxygen has two key roles in the sensitivity of ZnO towards HCHO: (1) it leads to the presence of charge trap states, which vanish upon the adsorption of HCHO, and (2) it facilitates the dissociative chemisorption of HCHO on the surface.

Reactive Oxygen Species Sequestration Induced Synthesis of β-PbO and Its Polymorphic Transformation to α-PbO at Atomically Thin Regimes.

The emergence of attractive properties in materials at atomically thin regimes has seen an ongoing interest in two-dimensional (2D) materials. An aspect that has lacked focused attention is the effect of 2D material thickness on its crystal structure. As several layered materials naturally exist in mixed metastable phases, it raises an important question of whether a specific polymorph of these mixed-phase materials will be favored at atomically thin limits.

Large Area Ultrathin InN and Tin Doped InN Nanosheets Featuring 2D Electron Gases.

Indium nitride (InN) has been of significant interest for creating and studying two-dimensional electron gases (2DEG). Herein we demonstrate the formation of 2DEGs in ultrathin doped and undoped 2D InN nanosheets featuring high carrier mobilities at room temperature. The synthesis is carried out via a two-step liquid metal-based printing method followed by a microwave plasma-enhanced nitridation reaction.

Surface Functionalization of WS Nanosheets with Alkyl Chains for Enhancement of Dispersion Stability and Tribological Properties.

Tungsten disulfide (WS) exhibits intriguing tribological properties and has been explored as an excellent lubricious material in thin-film and solid lubricants. However, the poor dispersibility of WS has been a major challenge for its utilization in liquid lubricant applications. Herein, a top-down integrated approach is presented to synthesize oxygenated WS (WS-O) nanosheets strong acid-mediated oxidation and ultrasound-assisted exfoliation.

Tuning the Schottky barrier height in a multiferroic InSe/FeGeTe van der Waals heterojunction.

The ferroelectric material InSe is currently of significant interest due to its built-in polarisation characteristics that can significantly modulate its electronic properties. Here we employ density functional theory to determine the transport characteristics at the metal-semiconductor interface of the two-dimensional multiferroic InSe/FeGeTe heterojunction. We show a significant tuning of the Schottky barrier height as a result of the change in the intrinsic polarisation state of InSe: the switching in the electric polarisation of InSe results in the switching of the nature of the Schottky barrier, from being n-type to p-type, and is accompanied by a change in the spin polarisation of the electrons.

Nicotine Sensors for Wearable Battery-Free Monitoring of Vaping.

Nicotine, an addictive substance in tobacco products and electronic cigarettes (e-cigs), is recognized for increasing the risk of cardiovascular and respiratory disorders. Careful real-time monitoring of nicotine exposure is critical in alleviating the potential health impacts of not just smokers but also those exposed to second-hand and third-hand smoke. Monitoring of nicotine requires suitable sensing material to detect nicotine selectively and testing under free-living conditions in the standard environment.

Fully Light-Controlled Memory and Neuromorphic Computation in Layered Black Phosphorus.

Imprinting vision as memory is a core attribute of human cognitive learning. Fundamental to artificial intelligence systems are bioinspired neuromorphic vision components for the visible and invisible segments of the electromagnetic spectrum. Realization of a single imaging unit with a combination of in-built memory and signal processing capability is imperative to deploy efficient brain-like vision systems.

Liquid-Metal Synthesized Ultrathin SnS Layers for High-Performance Broadband Photodetectors.

Atomically thin materials face an ongoing challenge of scalability, hampering practical deployment despite their fascinating properties. Tin monosulfide (SnS), a low-cost, naturally abundant layered material with a tunable bandgap, displays properties of superior carrier mobility and large absorption coefficient at atomic thicknesses, making it attractive for electronics and optoelectronics. However, the lack of successful synthesis techniques to prepare large-area and stoichiometric atomically thin SnS layers (mainly due to the strong interlayer interactions) has prevented exploration of these properties for versatile applications.

Structural-Defect-Mediated Grafting of Alkylamine on Few-Layer MoS and Its Potential for Enhancement of Tribological Properties.

Two-dimensional transition-metal dichalcogenides possess inherent structural characteristics that can be harnessed for enhancement of tribological properties by making them dispersible in lube media. Here, we present a hydrothermal approach to preparing MoS nanosheets comprising 4-10 molecular lamellae. A structural-defect-mediated route for grafting of octadecylamine (ODA) on MoS nanosheets is outlined.

Electrically Activated UV-A Filters Based on Electrochromic MoO.

Chromism-based optical filters is a niche field of research, due to there being only a handful of electrochromic materials. Typically, electrochromic transition metal oxides such as MoO and WO are utilized in applications such as smart windows and electrochromic devices (ECD). Herein, we report MoO-based electrically activated ultraviolet (UV) filters.

Differential Work-Function Enabled Bifunctional Switching in Strontium Titanate Flexible Resistive Memories.

Multifunctional electronic memories capable of demonstrating both analog and digital switching on-demand are extremely attractive for miniaturization of electronics without significant drain on energy consumption. Simultaneously translating functionality onto mechanically conformable platforms will further enhance their suitability. Here, we demonstrate the ability to engineer multifunctionality in strontium titanate (STO)-based resistive random-access memories (ReRAM) on a flexible polyimide platform.

Theoretical insight on the origin of anelasticity in zinc oxide nanowires.

Anelasticity of nanowires has recently attracted attention as an interesting property for high efficiency mechanical damping materials. While the mechanism of anelasticity has so far been analysed using continuum mechanical models based on defect diffusion, the mechanisms behind anelasticity have not yet been determined on an atomic level. Such information is needed in order to be able to design and synthesise new nanomaterials having desired mechanical properties.

Electronic transport investigation of redox-switching of azulenequinones/hydroquinones via first-principles studies.

The redox switching of non-alternant azulenequinone/hydroquinone molecules is investigated using density functional theory and the nonequilibrium Green's function. We examined the electronic transport properties of these molecules when subtended between gold electrodes. The results indicated that the reduction of 1,5-azulenequinone and oxidation of 1,7-azulene hydroquinone 2,6-dithiolate lead to a significant enhancement of the current compared to the respective oxidation of 1,5-azulene hydroquinone and reduction of 1,7-azulenequinone, thus "switching on" the transmission.

Adsorption of toxic gases on silicene/Ag(111).

Silicene is a two-dimensional nanomaterial, composed of Si atoms arranged into a buckled honeycomb network. It has become of great interest in recent years due to its remarkable properties such as its natural compatibility with current silicon-based technology. Due to its extreme thinness on the nanoscale, and large lateral dimensions, it has potential applications in gas sensing, gas storage and components in modern electronic devices.

Photochemical Etching of Carbonyl Groups from a Carbon Matrix: The (001) Diamond Surface.

The surface of diamond is reported to undergo nonablative photochemical etching when exposed to ultraviolet (UV) radiation which allows controlled single and partial layer removal of lattice layers. Oxygen termination of surface dangling bonds is known to be crucial for the etching process; however, the exact mechanism of carbon ejection remains unclear. We investigate the interaction of UV laser pulses with oxygen-terminated diamond surfaces using atomic-scale surface characterization combined with first-principles time-dependent density functional theory calculations.

Electrically Sorted Single-Walled Carbon Nanotubes-Based Electron Transporting Layers for Perovskite Solar Cells.

Incorporation of as prepared single-walled carbon nanotubes (SWCNTs) into the electron transporting layer (ETL) is an effective strategy to enhance the photovoltaic performance of perovskite solar cells (PSCs). However, the fundamental role of the SWCNT electrical types in the PSCs is not well understood. Herein, we prepared semiconducting (s-) and metallic (m-) SWCNT families and integrated them into TiO photoelectrodes of the PSCs.

Tuning the work function of the silicene/4 × 4 Ag(111) surface.

Silicene, the silicon analog of graphene, is an atomically thin two-dimensional material with promising applications in gas sensing, storage and as components in modern electronic devices. Silicene epitaxially grown on the Ag(111) surface can expand the utility of the silver surface by enabling the tuning of its work function through the functionalisation of silicene. Here we examine the electronic and structural properties and the thermodynamic stability of functionalised silicene/4 × 4 Ag(111) using density functional theory calculations coupled with ab initio molecular dynamics (AIMD) simulations.

van der Waals forces control ferroelectric-antiferroelectric ordering in CuInPS and CuBiPSe laminar materials.

We show how van der Waals (vdW) forces outcompete covalent and ionic forces to control ferroelectric ordering in CuInPS nanoflakes as well as in CuInPS and CuBiPSe crystals. While the self-assembly of these 2D layered materials is clearly controlled by vdW effects, this result indicates that the internal layer structure is also similarly controlled. Using up to 14 first-principles computational methods, we predict that the bilayers of both materials should be antiferroelectric.

Superconductivity in intercalated buckled two-dimensional materials: KGe.

Germanene has emerged as a novel two-dimensional material with various interesting properties and applications. Here we report the possibility of superconductivity in a stable potassium intercalated germanene compound, KGe2, with a transition temperature Tc ∼ 11 K, and an electron-phonon coupling of 1.9.