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Schematic (a) and cross-section (b) of the Np fabrication flow-cell design comprising of base (1), target material (2), laser window (3), gasket (4), top-plate (5) and O-ring (6)

Schematic (a) and cross-section (b) of the Np fabrication flow-cell design comprising of base (1), target material (2), laser window (3), gasket (4), top-plate (5) and O-ring (6)

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Nanotechnology is a significant research tool for biological and medical research with major advancements achieved from nanoparticle (Np) applications in biosensing and biotherapeutics. For laser ablation synthesis in solution (LASiS) to be chosen by researchers for Np colloid production, the process must effectively compete with chemical synthesis...

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... Different approaches have been carried out to fabricate Si nanoparticles, however, the laser ablation of a solid target immersed in a liquid, has shown to be an excellent alternative to fabricate colloidal Si nanoparticles [9,[11][12][13][14][15][16][17] due to its ability to produce hazardous waste free suspensions and nanoparticles with low size polydispersity [18]. As compared to chemical routes for the synthesis of nanoparticles in which chemical precursors, stabilizers and surfactants are used, the laser ablation of solids in liquids offers the advantage of obtaining pure nanoparticles without generation of residues arising from all chemicals used for reactions [19][20][21], avoiding the need for washing procedures for the final products. ...
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Colloidal silicon nanoparticle suspensions have been synthesized by the laser ablation of solids in liquids technique. We employed a picosecond laser to irradiate a silicon wafer immersed into distilled water at different fluences. After 30 months of aging, the optical properties of the nanoparticle suspensions were studied by photoluminescence spectroscopy, revealing the existence of visible light emissions arising from quantum confinement effects due to size reduction. Raman microspectroscopy was used to further observe size reduction of Si by analyzing shifts to lower frequencies of the Si-Si main vibrational mode associated to quantum confinement of phonons in silicon at nanoscale dimensions. Transmission electron microscopy measurements corroborated the presence of Si nanoparticles in the suspensions. Furthermore, the stability of these aged nanoparticles was confirmed by measuring their zeta potential. Results are analyzed and discussed in terms of the influence of the per pulse laser fluence on the nanoparticle features.
... Here, inspired by such successes of laser nanofabrication we leverage several emerging methods (building upon our previous work 21 ) to prepare a nanostructured biosensor, aiming to confer the advantages of laser-based fabrication onto biosensor fabrication, advancing the field towards the goals of producing inexpensive biosensors in abundance. The methods used were continuous flow Laser Ablation Synthesis in Solution (LASiS) 22,23 and Confined Atmospheric Pulsed-laser deposition (CAP) 24,25 . A schematic of sensor fabrication process is shown in Fig. 1. ...
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The advancement of biosensor research has been a primary driving force in the continuing progress of modern medical science. While traditional nanofabrication methods have long been the foundation of biosensor research, recent years have seen a shift in the field of nanofabrication towards laser-based techniques. Here we report a gold-based biosensor, with a limit of detection (LoD) 3.18 µM, developed using environmentally friendly Laser Ablation Synthesis in Liquid (LASiS) and Confined Atmospheric Pulsed-laser (CAP) deposition techniques for the first time. The sensors were able detect a DNA fragment corresponding to the longest unpaired sequence of the c-Myc gene, indicating their potential for detecting such fragments in the ctDNA signature of various cancers. The LoD of the developed novel biosensor highlights its reliability and sensitivity as an analytical platform. The reproducibility of the sensor was examined via the production and testing of 200 sensors with the same fabrication methodology. This work offers a scalable, and green approach to fabricating viable biosensors capable of detecting clinically relevant oncogenic targets.
... From Figure 2d, it can also be observed that no secondary peaks were observed for all the nanoparticles produced USP and by LASiS operated under batch and recirculation mode. The absence of secondary peaks shows the stability of AgNPs in the solution [21]. Figure 3 shows the zeta-potential (ξ) measurements of the as-produced LASiS AgNPS colloid in DI water. ...
... Size dispersion of the nanoparticle colloids was analysed using NanoFlex dynamic light scattering (DLS) analysis (Microtrac Inc., Hann, Germany.) using five acquisitions For batch LASiS, the target material was placed in a beaker and submerged in 4 mL of DI water. For recirculatory flow LASiS, an in-house designed polymer 3D-printed flow cell described, previously described in the literature contained the target material [19][20][21]. A peristaltic pump (Millipore Ltd., Burlington, VT, USA) was used to maintain a recirculating flow of DI-water over the AG target surface at 100 mL min −1 . ...
... Size dispersion of the nanoparticle colloids was analysed using NanoFlex dynamic light scattering (DLS) analysis (Microtrac Inc., Hann, Germany.) using five acquisitions per 30 s [21]. The nanoparticle size and morphology were analysed using a Philips CM20 TEM operated at 200 kV. ...
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... As a result, the laser ablation technique cannot currently achieve all of the advantages of chemical methods, and more effort is required to produce better nanoparticles [9]. In recent years, the productivity of laser ablated nanoparticle production has been improved by introducing dynamic flow based laser ablation [89][90][91][92][93]. The target material was submerged in a dynamic liquid, which minimizes the likelihood of laser pulse attenuation due to ablated nanoparticle accumulation. ...
... The target material was submerged in a dynamic liquid, which minimizes the likelihood of laser pulse attenuation due to ablated nanoparticle accumulation. Freeland et al. achieved very efficient laser ablation of silicon nanoparticles within a flow cell in a laminar flow environment [89]. They increased the yield of nanoparticles by optimising the flow parameters within the flow cell. ...
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... The produced colloids were characterized using UV-VIS Spectrophotometer (Biochrom Inc., USA, scan range 200-1200 nm with scan rate 600 nm min -1 ) (Fig. 2) to confirm nanoparticle formation. The absorption peaks in the 400 nm wavelength region confirm silver nanoparticle formation under the experimental conditions: pulse repletion rate, fPRF = 20 kHz, process duration, t=30 min, and laser bean scan speed, v =2.2 mm s -1 in DI water [39]. The inset of Fig. 2 shows a picture of LASiS silver nanocolloids produced for the corresponding UV-VIS spectra. ...
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Silver nano-colloids have been generated via Laser Ablation Synthesis in Solution (LASiS) system. Nanoparticle formation with particle size below 50 nm in DI water was confirmed using UV-VIS spectroscopy, Dynamic Light Scattering (DLS) technique, and transmission electron microscopy (TEM). Supercapacitor structure, having dimension 11 mm x 10 mm, was successfully Aerosol Jet printed on an untreated polymer substrate using as produced LASiS silver nano-colloid.
... All these factors, especially NP productivity and concentration, strongly affect the conductivity of the print pattern achievable with conductive inks and thereby the quality of PE devices. To overcome such challenges, several approaches, including a selection of appropriate liquid and level of liquid, laser parameter optimization, and static and dynamic flow-based methods, have been reported [58][59][60][61]. In this work, we report, the high yield additive-free Ag NP ink development using LASiS and its Aerosol Jet printing for the first time with excellent printing efficiency and spatial uniformity. ...
... The peristaltic pump controls the flow rate of the DI water through the PTFE pipping network which can provide the liquid flow rate 10 mL min -1 -400 mL min -1 . The top part of the flow-cell was fabricated using VeroWhitePlus (RGD835) photopolymer and the bottom part was printed using the photopolymer TangoBlack (FLX973) and it was additively developed in Stratasys Connex1 Polyjet 3D printer[61,68]. The flow-cell consists of a bottom plate, quartz laser window, rubber O-ring, Ag target and top part[61]. Process parameters such as, laser power (W), stage height (mm), v (mm sec -1 ), raster pattern(Fig. ...
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... This is a very simple technique to perform, but it is quite inefficient with low NP productivity. In this work, we build upon the flow ablation process developed by Streubel et al. [21] and Waag et al. [22], while using both the flow-cell design and recirculation configuration reported by Freeland et al. [23,14], to recirculate liquid over the target in a controlled manner to create a novel enhanced PLAL system. In doing so, the SiNPs are directed away from the ablation site, reducing the laser shielding effects created by the produced NPs, and allowing for significantly larger colloid production volumes and concentrations. ...
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Hypothesis Functionalized nanoparticles (NPs) offer diverse biomedical applications, but their synthesis is complex, costly, and labour-intensive, particularly when providing for additional functionalization requirements which are a key feature of biomedical applications. Pulsed laser ablation in liquids (PLAL) has previously allowed for the synthesis of metal and metal oxide nanoparticles using metal targets, which can then be surface functionalized during synthesis by the surrounding liquid species. Therefore, it should be possible to achieve biomolecule functionalization by ablating in biomolecular solutions. We explore a novel controlled recirculation PLAL scheme which should increase functionalization and productivity of functionalized nanoparticles. Experiments Traditional PLAL was performed by ablating a silicon target in a DNA solution. We have extended beyond traditional approaches by ablating the silicon target under novel flow conditions in a controlled recirculating loop of DNA solution. Findings Ablating in a DNA solution allows for high efficiency binding of DNA to silicon nanoparticles (SiNPs) in a single step process. By using SiNPs we are significantly reducing the overall cost of the process, when compared with the more traditional use of gold or silver; as well as, using a biocompatible material with an affinity for protein and nucleic acid binding. Reducing the laser shielding effects of particles and debris by removing them from the ablation site produces higher volumes and concentrations of functionalized colloid. Recirculating this liquid over the target has resulted in a 50% relative increase in binding efficiency, compared with static and single-pass flow conditions processing, achieving an average maximum binding efficiency of 78% in flow compared to 52% under static conditions. Furthermore, by reducing the initial DNA concentration, we were able to achieve 100% binding efficiency, which we believe to be the highest reported in literature to date.
... In 1987, Patil et al. first explored material synthesis at a solidliquid interface using a pulsed laser (ruby laser with a pulse width of 30 ns) by generating metastable iron oxide from an iron substrate in water [23]. Later in 1993, Neddersen et al. reported the generation of organic solvent and water based stable colloids, without any ionic or organic species, from metal targets such as Cu, Pt, Pd, Au and Ag via laser ablation [24]. The LASiS technique has been used for the generation of highly pure nanostructures in aqueous solutions at room temperature and normal pressure conditions since 2000 [14,[25][26][27][28] and several NP colloids of metals (e.g., Ag [29], Cu [29,30] and Au [31]), polymers [32], semiconductors (e.g., silicon carbide (SiC) [33], silicon (Si) [34] and zinc oxide (ZnO) [35]) and carbon (C) [36] have been synthesized using this method. ...
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Conductive inks allow for low cost and scalable deposition of conductive tracks and patterns for printed electronics. Metal nanoparticle colloids are a novel form for producing conductive inks. Laser Ablation Synthesis in Solution (LASiS) is a “green” method for the production of metal nanoparticle colloids without the need for environmentally hazardous chemicals, however the method has typically been limited by its low production rates. This study reports on the generation of an additive free silver nanocolloid with maximized productivity using a flow-based LASiS system and its characterization using dynamic light scattering, UV–VIS, transmission electron microscopy and field emission scanning electron microscopy. The productivity of the LASiS silver nanoparticle (size ∼34 ± 5 nm) was ∼0.9 mg mL⁻¹. While the flow-based system achieves high laser ablation rates in the mass of nanomaterial generated per unit time, the volume of liquid required for the flow leads to relatively low concentrations. Therefore, in this work, LASiS concentrated ink was formulated via a centrifugal method, which was then drop-cast and heat treated to produce a conductive silver layer. Centrifuging to concentrate the ink was shown to be a necessary step to achieve good results, with the lowest resistance across the drop-cast material of 60.2 Ω after annealing.