Gold Nanoparticle Networks Research Articles

Physical reservoir application of random network of gold nanoparticles fabricated by multi-step immersion in gold colloidal solution

We fabricated a random network of gold nanoparticles (RN-GNPs) over 12 NiCr/Au electrodes by using a multi-step immersion method, where a sample was immersed in a gold colloid solution three times. Nonlinear current–voltage characteristics due to the Coulomb blockade were observed at 77 K. For demonstration of physical reservoir applications, input–output characteristics of the RN-GNPs were also measured in a one-input, nine-output terminal configuration. Distorted output voltage waveforms were obtained for a sinusoidal voltage input of 100 Hz. The higher-order harmonic components were confirmed in the frequency spectra of the outputs. The waveform reconstruction task and short-term storage capacity estimation were performed by an echo state network model with ridge regression and linear regression, respectively.

A kinetic Monte Carlo approach for Boolean logic functionality in gold nanoparticle networks

Nanoparticles interconnected by insulating organic molecules exhibit nonlinear switching behavior at low temperatures. By assembling these switches into a network and manipulating charge transport dynamics through surrounding electrodes, the network can be reconfigurably functionalized to act as any Boolean logic gate. This work introduces a kinetic Monte Carlo-based simulation tool, applying established principles of single electronics to model charge transport dynamics in nanoparticle networks. We functionalize nanoparticle networks as Boolean logic gates and assess their quality using a fitness function. Based on the definition of fitness, we derive new metrics to quantify essential nonlinear properties of the network, including negative differential resistance and nonlinear separability. These nonlinear properties are crucial not only for functionalizing the network as Boolean logic gates but also when our networks are functionalized for brain-inspired computing applications in the future. We address fundamental questions about the dependence of fitness and nonlinear properties on system size, number of surrounding electrodes, and electrode positioning. We assert the overall benefit of having more electrodes, with proximity to the network’s output being pivotal for functionality and nonlinearity. Additionally, we demonstrate an optimal system size and argue for breaking symmetry in electrode positioning to favor nonlinear properties.

Heat Transfer Enhancement in Tree-Structured Polymer Linked Gold Nanoparticle Networks.

Human brains use a tree-like neuron network for information processing at high efficiency and low energy consumption. Tree-like structures have also been engineered to enhance mass and heat transfer in various applications. In this work, we reveal the heat transfer mechanism in tree-structured polymer linked gold nanoparticle (AuNP) networks using atomistic simulations. We report both upward and downward heat fluxes between root and leaf nodes in tree-structured polyethylene (PE) and poly(p-phenylene) (PPP) linked AuNP networks at tree levels from 1 to 5. We found that the heat conductance increases with an increasing polymer tree level. The heat transfer enhancement is due to the resulting increase in the low-frequency vibrational modes. This and other thermal properties are affected by the location of the AuNPs in the tree. Moreover, complex tree structures with at least five levels were found to be robust in the sense that disabling half of the leaves did not change the overall heat conductance.

Fractal-like gold nanonetworks formed by templated electrodeposition through 3D-mesoporous silica films.

Fractal-like networks of gold nanoparticles created by templated electrodeposition are described. Templated electrodeposition is a powerful and efficient technique for the bottom-up fabrication of nanostructures which can effectively control the size and shape of the electrodeposits. In this work, mesoporous silica films with highly ordered mesopores and three-dimensional mesostructure are synthesised and are used as templates for the electrodeposition of gold nanoparticles. The mesoporous silica films have small mesopores (∼8 nm) and complex mesopore channels (Fmmm structure with the [0 1 0] axis perpendicular to the substrate). A variety of nucleation conditions were applied to investigate their effect on the nanoparticles' arrangement and growth in templated electrodeposition. The electrodeposited gold particles are characterised by electron microscopy and grazing incidence small-angle X-ray scattering (GISAXS). GISAXS shows changes in the lattice parameters of the mesostructure after gold electrodeposition that relate to dimensional changes in directions linked to the shortest distances between the main spherical pores. Top-view SEM shows large areas of gold nanoparticles were deposited into the film and they were growing towards the surface. After removing the silica film templates, the gold nanoparticles display interesting fractal morphologies: the linked gold nanonetworks form a branched structure. The lengths of branches vary from the applied nucleation deposition conditions. Generally, with increasing nucleation time, fractal gold nanoparticles with longer branches are more likely to be obtained.

Nanoparticle‐Based Strain Gauges: Anisotropic Response Characteristics, Multidirectional Strain Sensing, and Novel Approaches to Healthcare Applications

AbstractDirectional strain sensing is essential for advanced sensor applications in the field of human‐machine interfaces and healthcare. Here, the angle dependent anisotropic strain sensitivity caused by charge carriers percolating through cross‐linked gold nanoparticle (GNP) networks is studied and these versatile materials are used for the fabrication of wearable triaxial pulse and gesture sensors. More specifically, the anisotropic response of 1,9‐nonanedithiol cross‐linked GNP films is separated into geometric and piezoresistive contributions by fitting the measured data with an analytic model. Hereby, piezoresistive coefficients of g11 ∼ 32 and g12 ∼ 21 are extracted, indicating a slightly anisotropic response behavior of the GNP‐based material. To use the material for healthcare applications, arrangements of three GNP transducers are patterned lithographically and fully embedded into a highly flexible silicone polymer (Dragon Skin 30). The new encapsulation method ensures good and robust electrical contacts and enables facile handling and protection from external influences. A facile read‐out with wireless data transmission using off‐the‐shelf electrical components underlines the great potential of these devices for applications as skin‐wearable healthcare sensors.

Arsenic ion assisted core–satellites nano-assembly of gold nanoparticles for its colorimetric determination in water

Arsenic contamination in water has threatened lives globally. The capability of arsenic to interact with the sulfhydryl group of amino acids in human body is considered as one of the factors leading to its increased toxicity and there is the dire need for development of better detection platforms. In this study, advantage of natural biomimetic interaction between thiol rich ligands and arsenic ions along with the effect of nanoarchitecture was evaluated by fabricating a heterostructural bioreceptor probe which interacts with arsenic based on affinity interaction to bring about a visual colorimetric response via plasmon coupling. As (III) ions can bind to these selective ligands and self-assemble to form gold nanoparticle networks. The mesh-like nanoarchitecture enhances the available surface area for interaction between selective bioreceptor heads and As (III) ions. The developed chemoprobe was validated by assessing the spiked real water samples with recoveries of 95–103%. The results indicate that the chemical nanoprobe was responsive over a wide linear range of 1 to 200 μg L−1, offering the detection limit of 0.22 μg L−1 and selective for As (III) ions in a presence of 10 times more concentrated solution of the competing ions which indicates at the potential of nano-architecture in improving current detection systems.

Voltammetric sensing of recombinant viral dengue virus 2 NS1 based on Au nanoparticle\u2013decorated multiwalled carbon nanotube composites

A homemade gold electrode is modified with a carbon nanotubes/gold nanoparticles nanocomposite to perform selective and sensitive electrochemical detection of dengue toxin. This nanostructured composite offers a large specific surface and a reactive interface allowing the immobilization of biological material. Dengue antibodies are immobilized on gold nanoparticles via covalent bonding for dengue toxin detection. The porous tridimensional network of carbon nanotubes and gold nanoparticles enhances the electrochemical signal and the overall performance of the sensor. After optimization, the system exhibits a high sensitivity of − 0.44 ± 0.01 μA per decade with wide linear range between 1 × 10−12 and 1 × 10−6 g/mL at a working potential of 0.22 V vs Ag/AgCl. The extremely low detection limit (3 × 10−13 g/mL) ranks this immunosensor as one of the most efficient reported in the literature for the detection of recombinant viral dengue virus 2 NS1. This biosensor also offers good selectivity, characterized by a low response to various non-specific targets and assays in human serum. The outstanding performances and the reproducibility of the system place the biosensor developed among the best candidates for future medical applications and for early diagnosis of dengue fever.Graphical abstract

Amplified electrochemical determination of UO22+ based on the cleavage of the DNAzyme and DNA-modified gold nanoparticle network structure.

A superior electrochemical biosensor was designed for the determination of UO22+ in aqueous solution by integration of DNAzyme and DNA-modified gold nanoparticle (DNA-AuNP) network structure. Key features of this method include UO22+ inducing the cleavage of the DNAzyme and signal amplification of DNA-AuNP network structure. In this electrochemical method, the DNA-AuNP network structure can be effectively modified on the surface of gold electrode and then employed as an ideal signal amplification unit to generate amplified electrochemical response by inserting a large amount of electrochemically active indicator methylene blue (MB). In the presenceof UO22+, the specific sites on DNA-AuNP network structure can be cleaved by UO22+, releasing the DNA-AuNP network structure with detectable reduction of electrochemical response intensity. The electrochemical response intensity isrelated to the concentration of UO22+. The logarithm of electrochemical response intensity and UO22+ concentration showed a wide linear range of 10~100pM, and the detection limit reached 8.1pM (S/N = 3). This method is successfully used for determination of UO22+ in water samples. Graphical abstract Fabricated DNAzyme network structure for enhanced electrical signal. Numerical experiments show that the current signal decreases as the concentration of UO22+ increases. It can be seen that the biosensors could be used to detect UO22+ in aqueous solution effectively.

Negative Differential Resistance and Hysteresis in Self‐Assembled Nanoscale Networks with Tunable Molecule‐to‐Nanoparticle Ratios

Electronic transport is investigated through self‐assembled benzenedithiol–gold nanoparticle networks with tunable molecule‐to‐particle ratios (1:5–50:1) deposited between planar electrodes. Two‐terminal current–voltage measurements of the networks display linear behavior at low bias, which is described using a circuit model that accounts for different network morphologies, tunable via molecule‐to‐nanoparticle ratio, and defects. At larger biases, nonlinear negative differential resistance and hysteresis behavior are observed for different molecular concentrations, which can be attributed to a combination of field‐assisted tunneling and charge trapping occurring in the nanoscale networks. The directed self‐assembly of benzenedithiol–metal nanoparticle molecular electronic networks is suggested for molecular integrated circuits in applications such as memory, switching, hardware security, and computing.

Molecular dynamics study of thermal properties of nanofluids composed of one-dimensional (1-D) network of interconnected gold nanoparticles

In this Letter, Equilibrium Molecular Dynamics (EMD) simulations were used to investigate the nanoparticle volume fraction-dependent thermal conductivity of nanofluids composed of one-dimensional (1-D) network of interconnected gold nanoparticles (IAuNPs) within the Green–Kubo formula. Thermal conductivities of nanofluids containing spherical AuNPs were also studied for comparison. The results showed that the 1D network shape of IAuNPs improves the nanofluid thermal conductivity better than the spherical shape of AuNP. The mechanism responsible for this finding is discussed using the Mean-Square-Displacement (MSD) analysis and the Radial-Distribution-Function (RDF).

Surface stress-based biosensor with stable conductive AuNPs network for biomolecules detection

Abstract The composite of gold and PDMS hold remarkable potential for surface stress-based biosensor applicaitons. However, the gold and PDMS in composite suffers from poor compatibility with each other and suppresses the performance of the biosensor. Here, we conduct two-step synthesis of the composite of gold and PDMS by in-situ reduction and glucose reduction of HAuCl4. The composite shows stable conductive gold nanoparticle network (SC-AuNW). In in-situ reduction, Au-seeds are embedded in PDMS surface. Furthermore, AuNPs are also generated inside the PDMS and enhance conductivity. The SC-AuNW plays a crucial role in tunneling conductivity of composite film and exhibits an excellent sensitivity to surface stress. We construct SC-AuNW-PDMS biosensors based on surface stress for glucose detection with a detection limit of 0.021 mM, high repeatability and specificity. Our research can promote the application of flexible conductive films in biosensors for disease diagnosis.

3D hybrid networks of gold nanoparticles: mechanoresponsive electrical humidity sensors with on-demand performances.

We have engineered macroscopic 3D porous networks of gold nanoparticles (AuNPs) chemically interconnected by di-thiolated ethylene glycol oligomers. The formation of such superstructures has been followed by means of UV-Vis spectroscopy by monitoring the aggregation-dependent plasmonic band of such nanomaterials. The controlled chemical tethering of the AuNPs with di-thiolated linkers possessing a well-defined contour length rules the interparticle distance. The use of ad-hoc linkers ensures charge transport via direct tunneling and the hygroscopic nature of the ethylene glycol backbone allows interaction with moisture. Upon interaction with water molecules from the atmosphere, our 3D networks undergo swelling reducing the tunnelling current passing through the system. By exploiting such a behavior, we have devised a new approach for the fabrication of electrical resistive humidity sensors. For the first time we have also introduced a new strategy to fabricate stable and robust devices by covalently attaching our 3D networks to gold electrodes. Devices comprising both 4 (TEG) or 6 (HEG) ethylene glycol repetitive units combined with AuNPs exhibited (i) unprecedentedly high response speed (∼26 ms), (ii) short recovery time (∼250 ms) in the absence of any hysteresis effect, and (iii) a linear response to humidity changes characterized by a highest sensitivity of 51 kΩ per RH(%) for HEG- and 500 Ω per RH(%) for TEG-based devices. The employed green solution processing in water and the extreme robustness of our 3D networks make them interesting candidates for the fabrication of sensors which can operate under extreme conditions and for countless cycles.

2D hybrid networks of gold nanoparticles: mechanoresponsive optical humidity sensors.

Plasmonic coupling is a fascinating phenomenon occurring between neighboring metal nanostructures. We report a straightforward approach to study such process macroscopically by fabricating 2D networks of gold nanoparticles, interconnected with responsive hygroscopic organic linkers. By controlling the humidity we tune the interparticle distance to reversibly trigger plasmonic coupling collectively over several millimeters.

Ordered Networks of Gold Nanoparticles Crosslinked by Dithiol‐Oligomers

AbstractControlled aggregation of nanoparticles into superlattices is a grand challenge in material science, where ligand based self‐assembly is the dominant route. Here, the self‐assembly of gold nanoparticles (AuNPs) that are crosslinked by water soluble oligo‐(ethylene glycol)‐dithiol (oEG‐dithiol) is reported and their 3D structure by small angle X‐ray scattering is determined. Surprisingly, a narrow region is found in the parameter space of dithiol linker‐length and nanoparticle size for which the crosslinked networks form short‐ranged FCC crystals. Using geometrical considerations and numerical simulations, the stability of the formed lattices is evaluated as a function of dithiol length and the number of connected nearest‐neighbors, and a phase diagram of superlattice formation is provided. Identifying the narrow parameter space that allows crystallization facilitates focused exploration of linker chemical composition and medium conditions such as thermal annealing, pH, and added solutes that may lead to superior and more robust crystals.

Dynamic‐ and Light‐Switchable Self‐Assembled Plasmonic Metafilms

AbstractLarge‐area dynamic switchable plasmonic metafilms composed of a network of gold nanoparticles (Au NPs) and the thermo‐responsive polymer poly(N‐isopropylacrylamide) (PNIPAM) are self‐assembled by casting Au@PNIPAM core–shell nanoparticles. These dense plasmonic films present an unusual optical behavior arising from the macroscale effective medium response of the film and the microscopic interactions of the gold nanoparticles. Such intensely colored plasmonic metafilms can be thermally actuated across large areas via direct heating, allowing extraction of the tuning of the effective dielectric permittivity of this metamaterial. By contrast, local plasmonic heating by illuminating the Au NPs in these metafilms enables sub‐second and highly reversible contraction of the plasmonic metafilms, capable of pumping water. This work provides a paradigm for switchable metafilms and metasurfaces that can be harnessed for different applications such as sensing, imaging optics, and image displays.

Electrocatalytic hydrogen production on GCE/RGO/Au hybrid electrode

We have prepared a nanocomposite hybrid film to produce a collaborative network of gold (Au) nanoparticles that are highly dispersed on reduced graphene oxide (RGO) sheets, and tested it for electrocatalytic hydrogen production. The RGO/Au nanocomposite film synthesized on glassy carbon electrode (GCE) allows significant improvements to the electron-transfer process. The Au nanoparticles decorated on the surface of graphene increases the electron density, which synergistically promote the adsorption of hydrogen atoms on the graphene sheets and consequently enhance the hydrogen evolution reaction (HER) activity. The surface properties of the composite was characterized by field-emission scanning electron microscopy (FE-SEM) and the electrocatalytical performances evaluated as-prepared electrocatalyst toward (HER) by linear sweep voltammetry (LSV), Tafel polarization curves and electrochemical impedance spectroscopy (EIS) analyses. The GCE/RGO/Au nanohybrid electrode exhibited good catalytic activity for HER with an onset potential of −0.3 V and a Tafel slope of 136 mV dec−1, achieving a current density of 10 mA cm−2 at an overpotential of −0.43 V.

Assembly Behavior of Organically Interlinked Gold Nanoparticle Composite Films: A Quartz Crystal Microbalance Investigation.

Thin films based on dodecylamine stabilized gold nanoparticles interlinked with different organic molecules are prepared by automatic layer-by-layer self-assembly in a microfluidic quartz crystal microbalance (QCM) cell, to obtain an in situ insight on the film formation by ligand/linker exchange reactions. The influence of interlinking functional groups and the length of the organic linker molecule on the assembly behavior is investigated. Alkyldithiols with different lengths are compared to alkyldiamines and alkylbisdithiocarbamates with a C8 alkylic molecular backbone. The stepwise layer-by-layer assembly occurs independently of the linker molecule, while the largest frequency changes always correspond to the gold nanoparticle step. During the solvent rinsing and ligand/linker exchange reaction step, the frequency is almost constant with slight increases or decreases dependent on the molar mass of the linker compared to the exchanged ligand. The assembly efficiency is higher for shorter molecules and for molecules with stronger interacting functional groups. The densities of the composite films are calculated from QCM data and independent thickness measurements. They reflect the higher fraction of organic material in the films comprising longer organic linkers. The plasmon resonance band of the gold nanoparticles in the final assemblies is measured with UV/vis spectroscopy. Band positions in films prepared from dithiols and diamines of comparable lengths are very similar, while the spectrum of the bisdithiocarbamate film exhibits a distinct blue-shift. This observation is explained by the longer molecular structure of the linker due to a larger binding group, in conjunction with a delocalization of particle charge on the organic molecule. Obtained results play an essential role in the understanding of thin film layer-by-layer self-assembly processes, and enable the formation of new gold nanoparticle networks with organic diamine and bisdithiocarbamate molecules.

Negative Differential Resistance, Memory, and Reconfigurable Logic Functions Based on Monolayer Devices Derived from Gold Nanoparticles Functionalized with Electropolymerizable TEDOT Units

We report on hybrid memristive devices made of a network of gold nanoparticles (10 nm diameter) functionalized by tailored 3,4(ethylenedioxy)thiophene (TEDOT) molecules, deposited between two planar electrodes with nanometer and micrometer gaps (100 nm to 10 um apart), and electropolymerized in situ to form a monolayer film of conjugated polymer with embedded gold nanoparticles (AuNPs). Electrical properties of these films exhibit two interesting behaviors: (i) a NDR (negative differential resistance) behavior with a peak/valley ratio up to 17, and (ii) a memory behavior with an ON/OFF current ratio of about 1E3 to 1E4. A careful study of the switching dynamics and programming voltage window is conducted demonstrating a non-volatile memory. The data retention of the ON and OFF states is stable (tested up to 24h), well controlled by the voltage and preserved when repeating the switching cycles (800 in this study). We demonstrate reconfigurable Boolean functions in multiterminal connected NP molecule devices.

One-step synthesis and self-assembly of a luminescent sponge-like network of gold nanoparticles with high absorption capacity

One-step strategy to fabricate a luminescent sponge-like network of AuNPs with a high capacity for heavy metal ion absorption.

Thermal transport enhancement in gold nanofluid containing network like structure

In this report, we have shown that gold nanofluid containing networked gold particles have much more enhancement (≈35%) in thermal transport in comparison to gold nanofluid containing conventional spherical gold nanoparticles under similar condition and loading fraction. This shows that structure or shape of the loading materials has very important effect on thermal conductivity of a nanofluid. Connected structure helps to increase the rate of heat transfer in the medium. The gold nanofluid having network of gold nanoparticles is synthesized in a single step process by pulsed laser ablation. The nanofluid (containing gold network) is stable and in addition to enhanced thermal conduction (compared to conventional gold nanofluids) shows no enhancement of viscosity unlike that seen in many nanofluids containing elongated nanomaterials (like cylinder or ellipsoids) in the dispersed phase which limits the use of nanofluids containing these kind of elongated structures in thermal transport though they have enhanced thermal conductivity than the conventional nanofluids (containing spherical nano particles). We synthesized and investigated the thermal transport in nanofluids containing network of Au nanoparticles instead of elongated nanomaterials in the dispersed phase as it retains the advantage of the spherical nanoparticles yet utilizes the enhanced heat transport by the network structure.