arXiv subjects

Jonathan N. Coleman

Publications and source records attributed to Jonathan N. Coleman.

15 recordsLinked to original sources

arXiv2025

Toward All 2D-based Printed Raindrop Triboelectric Nanogenerators

The raindrop triboelectric nanogenerator (RD-TENG) is an emerging technology that is designed to harvest energy from raindrops. This application requires materials with negative triboelectric effect, high surface charge density, mechanical flexibility, and a large surface area, which are key characteristics of 2D materials. However, fundamental research is necessary to understand the potential of 2D materials in this context. This study introduces all-2D-based RD-TENG devices using graphene and transition metal dichalcogenide (TMD) nanosheets. Liquid phase exfoliation (LPE) and liquid cascade centrifugation are used for nanosheet preparation and size selection. The TENGs are fabricated through a rapid, low-cost solution deposition technique based on liquid-liquid interface deposition, which allows screening of different active films and device geometries. Among the tested layered materials, medium-sized molybdenum disulfide (MoS2) nanosheets (average lateral size~160 nm, volume-fraction weighted average layer number ~9) exhibit the highest short-circuit current (microampere per drop) and voltage (mV per drop) output due to their most suited electron affinity, capacitance, and surface charge exchange properties. The variations in the performance of the TMD films were further evaluated with X-ray photoelectron spectroscopy (XPS), showing the influence of oxidation differences on charge transfer and charge decay time.

physics.app-ph↗

arXiv2025

Centrifugation theory revisited: Understanding and modelling the centrifugation of 2D nanosheets

Size selection of liquid-dispersed 2D nanomaterials is a prerequisite for size-dependent studies in earlier stage research and for their targeted application in commercial settings. Centrifugation is the most widespread method for reliably sorting suspensions of polydisperse 2D nanosheets according to size. However, whilst centrifugation is effective, no a priori models are available to predict the outcome of centrifugation, making time consuming iterative experiments necessary. Here we present a simple model for the behaviour of 2D nanosheets during centrifugation and benchmark its predictions against experiments. This model uses simple expressions, specific to 2D particles, for the hydrodynamic radius, effective density and viscous resistance to generate the equation of motion of individual nanosheet during centrifugation. Critically, the equation of motion is then used to predict nanosheet size distributions within centrifugation products. This in turn leads to equations for easily measurable properties such as mean and maximum nanosheet sizes obtained during centrifugation-based fractionation. Comparison with experimental data demonstrates the robustness of this model for a range of 2D materials and solvent systems, and its ability to describe quite subtle effects. These results will enable more tailored size selection of nanosheets for specific applications and offer new mechanistic insights to optimise exfoliation conditions.

cond-mat.mes-hall↗

arXiv2024

Using Electrical Impedance Spectroscopy to Separately Quantify the Effect of Strain on Nanosheet and Junction Resistance in Printed Nanosheet Networks

Many printed electronic applications require strain-independent electrical properties to ensure deformation-independent performance. Thus, developing printed, flexible devices using 2D and other nanomaterials will require an understanding of the effect of strain on the electrical properties of nano-networks. Here we introduce novel AC electrical techniques to fully characterise the effect of strain on the resistance of high mobility printed networks, fabricated from of electrochemically exfoliated MoS2 nanosheets. These devices were initially characterised using DC piezoresistance measurements and showed good cyclability and a linear strain response, consistent with a low gauge factor of G~3. However, AC impedance spectroscopy measurements, performed as a function of strain, allowed the measurement of the effects of strain on both the nanosheets and the inter-nanosheet junctions separately. The junction resistance was found to increase linearly with strain, while the nanosheet resistance remained constant. This response is consistent with strain-induced sliding of the highly-aligned nanosheets past one another, without any strain being transferred to the sheets themselves. Our approach allows us to individually estimate the contributions of dimensional factors (G~1.4) and intrinsic factors (G~1.9) to the total gauge factor. This novel technique may provide insight into other piezoresistive systems.

cond-mat.mes-hall↗

arXiv2024

Production of Ultra-Thin and High-Quality Nanosheet Networks via Layer-by-Layer Assembly at Liquid-Liquid Interfaces

Solution-processable 2D materials are promising candidates for a range of printed electronics applications. Yet maximising their potential requires solution-phase processing of nanosheets into high-quality networks with carrier mobility (μNet) as close as possible to that of individual nanosheets (μNS). In practise, the presence of inter-nanosheet junctions generally limits electronic conduction, such that the ratio of junction resistance (RJ) to nanosheet resistance (RNS), determines the network mobility via . Hence, achieving RJ/RNS<1 is a crucial step for implementation of 2D materials in printed electronics applications. In this work, we utilise an advanced liquid-interface deposition process to maximise nanosheet alignment and network uniformity, thus reducing RJ. We demonstrate the approach using graphene and MoS2 as model materials, achieving low RJ/RNS values of 0.5 and 0.2, respectively. The resultant graphene networks show a high conductivity of σNet = 5 \times 104 S/m while our semiconducting MoS2 networks demonstrate record mobility of μNet = 30 cm2/Vs, both at extremely low network thickness (tNet <10 nm). Finally, we show that the deposition process is compatible with non-layered quasi-2D materials such as silver nanosheets (AgNS), achieving network conductivity close to bulk silver for networks <100 nm thick. We believe this work is the first to report nanosheet networks with RJ/RNS<1 and serves to guide future work in 2D materials-based printed electronics.

cond-mat.mes-hall↗

arXiv2023

Quantifying the contribution of material and junction resistances in nano-networks

Networks of nanowires and nanosheets are important for many applications in printed electronics. However, the network conductivity and mobility are usually limited by the inter-particle junction resistance, a property that is challenging to minimise because it is difficult to measure. Here, we develop a simple model for conduction in networks of 1D or 2D nanomaterials, which allows us to extract junction and nanoparticle resistances from particle-size-dependent D.C. resistivity data of conducting and semiconducting materials. We find junction resistances in porous networks to scale with nanoparticle resistivity and vary from 5 Ohm for silver nanosheets to 25 GOhm for WS2 nanosheets. Moreover, our model allows junction and nanoparticle resistances to be extracted from A.C. impedance spectra of semiconducting networks. Impedance data links the high mobility (~7 cm2/Vs) of aligned networks of electrochemically exfoliated MoS2 nanosheets to low junction resistances of ~670 kOhm. Temperature-dependent impedance measurements allow us to quantitatively differentiate intra-nanosheet phonon-limited band-like transport from inter-nanosheet hopping for the first time.

cond-mat.mes-hall↗

arXiv2023

Knot Architecture for Biocompatible and Semiconducting Two-Dimensional Electronic Fibre Transistors

In recent years, the rising demand for close interaction with electronic devices has led to a surge in the popularity of wearable gadgets. While wearable gadgets have generally been rigid due to their utilisation of silicon-based technologies, flexible semiconducting fibre-based transistors will be needed for future wearables as active sensing components or within microprocessors to manage and analyse data. Two-dimensional (2D) semiconducting flakes are yet to be investigated in fibre transistors but could offer a route toward high-mobility, biocompatible and flexible fibre-based devices. Here we report the electrochemical exfoliation of semiconducting two-dimensional (2D) flakes of tungsten diselenide (WSe2) and molybdenum disulfide (MoS2). The high aspect ratio (>100) of the flakes achieves aligned and conformal flake-to-flake junctions on polyester fibres enabling transistors with mobilities ~ 1 cm^2 V^-1 s^-1 and a current on/off ratio, Ion/Ioff ~ 10^2 - 10^4. Furthermore, the cytotoxic effects of the MoS2 and WSe2 flakes with human keratinocyte cells are investigated and found to be biocompatible. As an additional step, we create a unique transistor knot architecture by leveraging the fibre diameter to establish the length of the transistor channel, facilitating a route to scale down transistor channel dimensions (100 μm) and utilise it to make MoS2 fibre transistors with a human hair that achieves mobilities as high as μ ~ 15 cm^2 V^-1 s^-1.

cond-mat.mtrl-sci↗

arXiv2023

3D-imaging of Printed Nanostructured Networks using High-resolution FIB-SEM Nanotomography

Networks of solution-processed nanomaterials are important for multiple applications in electronics, sensing and energy storage/generation. While it is known that network morphology plays a dominant role in determining the physical properties of printed networks, it remains difficult to quantify network structure. Here, we utilise FIB-SEM nanotomography to characterise the morphology of nanostructured networks. Nanometer-resolution 3D-images were obtained from printed networks of graphene nanosheets of various sizes, as well as networks of WS2 nanosheets, silver nanosheets and silver nanowires. Important morphological characteristics, including network porosity, tortuosity, pore dimensions and nanosheet orientation were extracted and linked to network resistivity. By extending this technique to interrogate the structure and interfaces within vertical printed heterostacks, we demonstrate the potential of this technique for device characterisation and optimisation.

cond-mat.mes-hall↗

arXiv2020

Equipartition of Energy Defines the Size-Thickness Relationship in Liquid-Exfoliated Nanosheets

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.

physics.chem-ph↗

arXiv2018

Spectroscopic size and thickness metrics for liquid-exfoliated h-BN

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.

cond-mat.mes-hall↗

arXiv2015

Mapping of Low-Frequency Raman Modes in CVD-Grown Transition Metal Dichalcogenides: Layer Number, Stacking Orientation and Resonant Effects

Layered inorganic materials, such as the transition metal dichalcogenides (TMDs), have attracted much attention due to their exceptional electronic and optical properties. Reliable synthesis and characterization of these materials must be developed if these properties are to be exploited. Herein, we present low-frequency Raman analysis of MoS2, MoSe2, WSe2 and WS2 grown by chemical vapour deposition (CVD). Raman spectra are acquired over large areas allowing changes in the position and intensity of the shear and layer-breathing modes to be visualized in maps. This allows detailed characterization of mono- and few-layered TMDs which is complementary to well-established (high-frequency) Raman and photoluminescence spectroscopy. This study presents a major stepping stone in fundamental understanding of layered materials as mapping the low-frequency modes allows the quality, symmetry, stacking configuration and layer number of 2D materials to be probed over large areas. In addition, we report on anomalous resonance effects in the low-frequency region of the WS2 Raman spectrum.

cond-mat.mtrl-sci↗

arXiv2015

Relating the optical absorption coefficient of nanosheet dispersions to the intrinsic monolayer absorption

The concentration of nanosheet suspensions is an important technological parameter which is commonly measured by optical spectroscopy using the absorption coefficient to transform absorbance into concentration. However for all 2D materials, the absorption coefficient is poorly known, resulting in potentially large errors in measured concentration. Here we derive an expression relating the optical absorption coefficient of an isotropic ensemble of nanosheets to the intrinsic monolayer absorption. This has allowed us to calculate the absorption coefficients for suspensions of graphene, MoS2 and other 2D materials and allows estimation of the monolayer absorption for new materials from careful measurement of the suspension absorption coefficient.

cond-mat.mes-hall↗

arXiv2015

Low wavenumber Raman spectroscopy of highly crystalline MoSe2 grown by chemical vapor deposition

Transition metal dichalcogenides (TMDs) have recently attracted attention due to their interesting electronic and optical properties. Fabrication of these materials in a reliable and facile method is important for future applications, as are methods to characterize material quality. Here we present the chemical vapor deposition of MoSe2 monolayer and few layer crystals. These results show the practicality of using chemical vapor deposition to reliably fabricate these materials. Low frequency Raman spectra and mapping of shear and layer breathing modes of MoSe2 are presented for the first time. We correlate the behavior of these modes with layer number in the materials. The usefulness of low frequency Raman mapping to probe the symmetry, quality, and monolayer presence in CVD grown 2D materials is emphasized.

cond-mat.mtrl-sci↗

arXiv2015

Liquid exfoliation of solvent-stabilised black phosphorus: applications beyond electronics

Few layer black phosphorus is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of stability severely limits our ability to synthesise and process this material. Here we demonstrate that high-quality, few-layer black phosphorus nanosheets can be produced in large quantities by liquid phase exfoliation in the solvent N-cyclohexyl-2-pyrrolidone (CHP). We can control nanosheet dimensions and have developed metrics to estimate both nanosheet size and thickness spectroscopically. When exfoliated in CHP, the nanosheets are remarkably stable unless water is intentionally introduced. Computational studies show the degradation to occur by reaction with water molecules only at the nanosheet edge, leading to the removal of phosphorus atoms and the formation of phosphine and phosphorous acid. We demonstrate that liquid exfoliated black phosphorus nanosheets are potentially useful in a range of applications from optical switches to gas sensors to fillers for composite reinforcement.

cond-mat.mes-hall↗

arXiv2014

Biocompatibility of Pristine Graphene Monolayers, Nanosheets and Thin Films

There is an increasing interest to develop nanoscale biocompatible graphene structures due to their desirable physicochemical properties, unlimited application opportunities and scalable production. Here we report the preparation, characterization and biocompatibility assessment of novel graphene flakes and their enabled thin films suitable for a wide range of biomedical and electronic applications. Graphene flakes were synthesized by a chemical vapour deposition method or a liquid-phase exfoliation procedure and then thin films were prepared by transferring graphene onto glass coverslips. Raman spectroscopy and transmission electron microscopy confirmed a predominantly monolayer and a high crystalline quality formation of graphene. The biocompatibility assessment of graphene thin films and graphene flakes was performed using cultured human lung epithelial cell line A549 employing a multimodal approach incorporating automated imaging, high content screening, real-time impedance sensing in combination with biochemical assays. No detectable changes in the cellular morphology or attachment of A549 cells growing on graphene thin films or cells exposed to graphene flakes (0.1 to 5 ug/mL) for 4 to 72 h was observed. Graphene treatments caused a very low level of increase in cellular production of reactive oxygen species in A549 cells, but no detectable damage to the nuclei such as changes in morphology, condensation or fragmentation was observed. In contrast, carbon black proved to be significantly more toxic than the graphene. These data open up a promising view of using graphene enabled composites for a diverse scope of safer applications.

q-bio.CB↗

arXiv2009

Graphene under hydrostatic pressure

In-situ high pressure Raman spectroscopy is used to study monolayer, bilayer and few-layer graphene samples supported on silicon in a diamond anvil cell to 3.5 GPa. The results show that monolayer graphene adheres to the silicon substrate under compressive stress. A clear trend in this behaviour as a function of graphene sample thickness is observed. We also study unsupported graphene samples in a diamond anvil cell to 8 GPa, and show that the properties of graphene under compression are intrinsically similar to graphite. Our results demonstrate the differing effects of uniaxial and biaxial strain on the electronic bandstructure.

cond-mat.mtrl-sci↗