Publications by authors named "John C de Mello"

Article Synopsis
  • Micro- and nano-plastics (MNPs) are harmful pollutants affecting ecosystems and human health, making their detection essential.
  • Thin gold films with a special array of nanogaps can effectively detect these tiny plastics using a technique called surface-enhanced Raman spectroscopy (SERS), which simplifies the sample prep process.
  • This method successfully identified specific types of micro-plastics in drinking water and wash-water from infant bottles, demonstrating its potential for environmental monitoring.
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Template-patterned, flexible transparent electrodes (TEs) formed from an ultrathin silver film on top of a commercial optical adhesive - Norland Optical Adhesive 63 (NOA63) - are reported. NOA63 is shown to be an effective base-layer for ultrathin silver films that advantageously prevents coalescence of vapor-deposited silver atoms into large, isolated islands (Volmer-Weber growth), and so aids the formation of ultrasmooth continuous films. 12 nm silver films on top of free-standing NOA63 combine high, haze-free visible-light transparency (T ≈ 60% at 550 nm) with low sheet-resistance ( ≈ 16 Ω sq), and exhibit excellent resilience to bending, making them attractive candidates for flexible TEs.

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Conjugated polymers are increasingly exploited for biomedical applications. In this work, we explored the optical characteristics of conjugated polymers of variable chemical structures at multiple levels relevant to biological interfacing, from fluorescence yield to their influence on cellular membrane potential. We systematically compared the performance of conjugated polymer as cast thin films and as nanoparticles stabilized with amphiphilic polyethylene glycol-poly lactic acid-co-glycolic acid (PEG-PLGA).

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We report a sensitive, fixed-wavelength, lock-in-based optical detector built from a light-emitting diode, two colour filters, a photodetector, a small number of discrete analogue components, and a low-cost microcontroller development board. We describe the construction, operating principle, use and performance of the optical detector, which may be used for both absorption and fluorescence measurements in either a 10-mm pathlength cuvette or a low-volume (<100 μl) flow-cell. For illustrative purposes the detector is applied here to a cholesterol assay based on the enzyme-mediated conversion of (non-emissive) Amplex Red into the fluorescent dye resorufin, providing a detection limit of 200 nM - some four orders of magnitude lower than the typical concentration of cholesterol in human serum.

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Squeezing light into nanometer-sized metallic nanogaps can generate extremely high near-field intensities, resulting in dramatically enhanced absorption, emission, and Raman scattering of target molecules embedded within the gaps. However, the scarcity of low-cost, high-throughput, and reproducible nanogap fabrication methods offering precise control over the gap size is a continuing obstacle to practical applications. Using a combination of molecular self-assembly, colloidal nanosphere lithography, and physical peeling, we report here a high-throughput method for fabricating large-area arrays of triangular nanogaps that allow the gap width to be tuned from ∼10 to ∼3 nm.

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Metallic nanogaps with metal-metal separations of less than 10 nm have many applications in nanoscale photonics and electronics. However, their fabrication remains a considerable challenge, especially for applications that require patterning of nanoscale features over macroscopic length-scales. Here, some of the most promising techniques for nanogap fabrication are evaluated, covering established technologies such as photolithography, electron-beam lithography (EBL), and focused ion beam (FIB) milling, plus a number of newer methods that use novel electrochemical and mechanical means to effect the patterning.

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Metallic nanogaps (MNGs) are fundamental components of nanoscale photonic and electronic devices. However, the lack of reproducible, high-yield fabrication methods with nanometric control over the gap-size has hindered practical applications. A patterning technique based on molecular self-assembly and physical peeling is reported here that allows the gap-width to be tuned from more than 30 nm to less than 3 nm.

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Metal halide perovskites (MHPs) have excellent optoelectronic and photovoltaic applications because of their cost-effectiveness, tunable emission, high photoluminescence quantum yields, and excellent charge carrier properties. However, the potential applications of the entire MHP family are facing a major challenge arising from its weak resistance to moisture, polar solvents, temperature, and light exposure. A viable strategy to enhance the stability of MHPs could lie in their incorporation into a porous template.

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Optogenetics combines optics and genetics to enable minimally invasive cell-type-specific stimulation in living tissue. For the purposes of bio-implantation, there is a need to develop soft, flexible, transparent and highly biocompatible light sources. Organic semiconducting materials have key advantages over their inorganic counterparts, including low Young's moduli, high strain resistances, and wide color tunability.

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Silicon nanowire (Si NW) sensors have attracted great attention due to their ability to provide fast, low-cost, label-free, real-time detection of chemical and biological species. Usually configured as field effect transistors (FETs), they have already demonstrated remarkable sensitivity with high selectivity (through appropriate functionalisation) towards a large number of analytes in both liquid and gas phases. Despite these excellent results, Si NW FET sensors have not yet been successfully employed to detect single molecules of either a chemical or biological target species.

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Gold is the most widely used electrode material for bioelectronic applications due to its high electrical conductivity, good chemical stability and proven biocompatibility. However, it adheres only weakly to widely used substrate materials such as glass and silicon oxide, typically requiring the use of a thin layer of chromium between the substrate and the metal to achieve adequate adhesion. Unfortunately, this approach can reduce biocompatibility relative to pure gold films due to the risk of the underlying layer of chromium becoming exposed.

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We report the influence of different polymer purification procedures on the photovoltaic performance of bulk heterojunction solar cells formed from binary blends of poly(3-hexylthiophene) (P3HT) and fullerenes. Selective Soxhlet extractions and metal scavenging agents were used to remove residual monomer, magnesium salt by-products and catalyst from high-weight P3HT (Mw 121 kg/mol, PDI 1.8, RR 99%) synthesised by the Grignard metathesis (GRIM) polymerization route.

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We report the use of a porous polytetrafluoroethylene capillary for the inline separation of liquid-liquid segmented flows, based on the selective wetting and permeation of the porous capillary walls by one of the liquids. Insertion of a narrow flow restriction at the capillary outlet allows the back pressure to be tuned for multiple liquid-liquid combinations and flow conditions. In this way, efficient separation of aqueous-organic, aqueous-fluorous and organic-fluorous segmented flows can be readily achieved over a wide range of flow rates.

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Here we show that the charge transfer (CT) absorption signal in bulk-heterojunction solar cell blends, measured by photothermal deflection spectroscopy, is directly proportional to the density of molecular donor:acceptor interfaces. Since the optical transitions from the ground state to the interfacial CT state are weakly allowed at photon energies below the optical gap of both the donor and acceptor, we can exploit the use of this sensitive linear absorption spectroscopy for such quantification. Moreover, we determine the absolute molar extinction coefficient of the CT transition for an archetypical polymer:fullerene interface.

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Rapid precipitation, immersion of a liquid formulation into a nonsolvent, is compared with drop casting for fabricating organic solar cells. Blends comprising poly-3-hexylthiophene (P3HT), phenyl-C61-butyric acid methyl ester (PCBM), and chlorobenzene were processed into bulk samples by using two distinct routes: rapid precipitation and drop casting. The resulting structure, phases, and crystallinity were analyzed by using small-angle neutron scattering, X-ray diffraction, differential scanning calorimetry, and muon spin resonance.

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The past decade has seen a steady rise in the use of microfluidic reactors for nanocrystal synthesis, with numerous studies reporting improved reaction control relative to conventional batch chemistry. However, flow synthesis procedures continue to lag behind batch methods in terms of chemical sophistication and the range of accessible materials, with most reports having involved simple one- or two-step chemical procedures directly adapted from proven batch protocols. Here we examine the current status of microscale methods for nanocrystal synthesis, and consider what role microreactors might ultimately play in laboratory-scale research and industrial production.

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Coplanar electrodes formed from asymmetric metals separated on the nanometre length scale are essential elements of nanoscale photonic and electronic devices. Existing fabrication methods typically involve electron-beam lithography--a technique that enables high fidelity patterning but suffers from significant limitations in terms of low throughput, poor scalability to large areas and restrictive choice of substrate and electrode materials. Here, we describe a versatile method for the rapid fabrication of asymmetric nanogap electrodes that exploits the ability of selected self-assembled monolayers to attach conformally to a prepatterned metal layer and thereby weaken adhesion to a subsequently deposited metal film.

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Channel-fouling is a pervasive problem in continuous flow chemistry, causing poor product control and reactor failure. Droplet chemistry, in which the reaction mixture flows as discrete droplets inside an immiscible carrier liquid, prevents fouling by isolating the reaction from the channel walls. Unfortunately, the difficulty of controllably adding new reagents to an existing droplet stream has largely restricted droplet chemistry to simple reactions in which all reagents are supplied at the time of droplet formation.

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We report the fabrication of efficient indium-tin-oxide-free organic solar cells based on poly(3-hexylthiophene-2,5-diyl):[6,6]-phenyl-C61-butyric acid methyl ester (P3HT:PCBM). All layers of the devices from the lowermost silver nanowire cathode to the uppermost conducting polymer anode are deposited from solution and processed at plastic-compatible temperatures<200 °C. Owing to the absence of an opaque metal electrode, the devices are semitransparent with potential applications in power-generating windows and tandem-cells.

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We study the appearance and energy of the charge transfer (CT) state using measurements of electroluminescence (EL) and photoluminescence (PL) in blend films of high-performance polymers with fullerene acceptors. EL spectroscopy provides a direct probe of the energy of the interfacial states without the need to rely on the LUMO and HOMO energies as estimated in pristine materials. For each polymer, we use different fullerenes with varying LUMO levels as electron acceptors, in order to vary the energy of the CT state relative to the blend with [6,6]-phenyl C61-butyric acid methyl ester (PCBM).

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We demonstrate a compact, low cost and practical fluorescence detection system for lab-on-a-chip applications. The system comprises a commercially available InGaN light emitting diode (501 nm) as light source, an organic or silicon photodiode detector, absorptive dye coated colour filters and linear and reflective polarisers. An injection moulded polystyrene microfluidic chip is used as the platform for fluorescence immunoassays for cardiac markers myoglobin and CK-MB.

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