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1.  Biocatalysts Immobilized in Ultrathin Ordered Films 
Sensors (Basel, Switzerland)  2010;10(11):10298-10313.
The immobilization of enzymes and other proteins into ordered thin materials has attracted considerable attention over the past few years. This research has demonstrated that biomolecules immobilized in different [Langmuir-Blodgett (LB)/Langmuir-Schaefer (LS)] matrixes retain their functional characteristics to a large extent. These new materials are of interest for applications as biosensors and biocatalysts. We review the growing field of oxidases immobilized onto ordered Langmiur-Blodgett and Langmuir-Schaefer films. Strategies for the preparation of solid supports and the essential properties of the resulting materials with respect to the envisaged applications are presented. Basic effects of the nature of the adsorption and various aspects of the application of these materials as biosensors, biocatalysts are discussed. Outlook of potential applications and further challenges are also provided.
doi:10.3390/s101110298
PMCID: PMC3230983  PMID: 22163470
biosensors; enzyme immobilization; Langmuir-Blodgett technique; enzyme activity; AFM
2.  Sensing Arrays Constructed from Nanoparticle Thin Films and Interdigitated Microelectrodes 
Sensors (Basel, Switzerland)  2006;6(6):667-679.
This paper describes the results of a study of a few design parameters influencing the performance of sensor arrays constructed from nanostructured thin films and interdigitated microelectrodes (IMEs). The nanostructured thin films on the IME devices were prepared from nonanedithiol (NDT) and mercaptoundecanoic acid (MUA) linked assemblies of 2-nm sized gold nanoparticles. The sensor array data in response to volatile organic compounds were collected and analyzed using fractional factorial experimental design and analysis of variance for understanding effects of the design parameters on the sensitivity. While the smaller value for the microelectrode space, width, and length generally led to higher response sensitivity, a strong dependence on the nature of the nanostructured thin films was found. The microelectrode space was the most important design parameter for NDT-based thin films. However, the microelectrode space, width, and length were found to play almost equally important roles for MUA-based thin films. The principal component analysis results for classification performances of the arrays consisting of a set of thin films have demonstrated the possibility of optimizing sensor arrays by appropriate selections of microelectrode parameters and nanostructured sensing films.
PMCID: PMC3874821
Sensing arrays; nanostructured thin films; volatile organic compounds; principal component analysis
3.  Promises and Challenges of Nanoplasmonic Devices for Refractometric Biosensing 
Nanophotonics  2013;2(2):83-101.
Optical biosensors based on surface plasmon resonance (SPR) in metallic thin films are currently standard tools for measuring molecular binding kinetics and affinities – an important task for biophysical studies and pharmaceutical development. Motivated by recent progress in the design and fabrication of metallic nanostructures, such as nanoparticles or nanoholes of various shapes, researchers have been pursuing a new generation of biosensors harnessing tailored plasmonic effects in these engineered nanostructures. Nanoplasmonic devices, while demanding nanofabrication, offer tunability with respect to sensor dimension and physical properties, thereby enabling novel biological interfacing opportunities and extreme miniaturization. Here we provide an integrated overview of refractometric biosensing with nanoplasmonic devices and highlight some recent examples of nanoplasmonic sensors capable of unique functions that are difficult to accomplish with conventional SPR. For example, since the local field strength and spatial distribution can be readily tuned by varying the shape and arrangement of nanostructures, biomolecular interactions can be controlled to occur in regions of high field strength. This may improve signal-to-noise and also enable sensing a small number of molecules. Furthermore, the nanoscale plasmonic sensor elements may, in combination with nanofabrication and materials-selective surface-modifications, make it possible to merge affinity biosensing with nanofluidic liquid handling.
doi:10.1515/nanoph-2012-0026
PMCID: PMC3804425  PMID: 24159429
Optical biosensors; refractometric sensors; surface plasmon resonance; plasmonics; figure of merit; single molecule detection; enzyme-linked biosensing; site-specific chemistry; supported lipid bilayer; pore-spanning lipid membrane; nanoparticle; nanohole; optofluidics
4.  Langmuir Films of Flexible Polymers Transferred to Aqueous/Liquid Crystal Interfaces Induce Uniform Azimuthal Alignment of the Liquid Crystal 
We reported recently that amphiphilic polymers can be assembled at interfaces created between aqueous phases and thermotropic liquid crystals (LCs) in ways that (i) couple the organization of the polymer to the order of the LC and (ii) respond to changes in the properties of aqueous phases that can be characterized as changes in the optical appearance of the LC. This investigation sought to characterize the behavior of aqueous-LC interfaces decorated with uniaxially compressed thin films of polymers transferred by Langmuir-Schaefer (LS) transfer. Here, we report physicochemical characterization of interfaces created between aqueous phases and the thermotropic LC 4-cyano-4’-pentylbiphenyl (5CB) decorated with Langmuir films of a novel amphiphilic polymer (polymer 1), synthesized by the addition of hydrophobic and hydrophilic side chains to poly(2-vinyl-4,4’-dimethylazlactone). Initial characterization of this system resulted in the unexpected observation of uniform azimuthal alignment of 5CB after LS transfer of the polymer films to aqueous-5CB interfaces. This paper describes characterization of Langmuir films of polymer 1 hosted at aqueous-5CB interfaces as well as the results of our investigations into the origins of the uniform ordering of the LC observed upon LS transfer. Our results, when combined, support the conclusion that uniform azimuthal alignment of 5CB is the result of long-range ordering of polymer chains in the Langmuir films (in a preferred direction orthogonal to the direction of compression) that is generated during uniaxial compression of the films prior to LS transfer. Although past studies of Langmuir films of polymers at aqueous-air interfaces have demonstrated that in-plane alignment of polymer backbones can be induced by uniaxial compression, these past reports have generally made use of polymers with rigid backbones. One important outcome of this current study is thus the observation of anisotropy and long-range order in Langmuir films of a novel flexible polymer. A second important outcome is the observation that the existence, extent, and dynamics of this order can be identified and characterized optically by transfer of the Langmuir film to a thin film of LC. Additional characterization of Langmuir films of two other flexible polymers [poly(methyl methacrylate) and poly(vinyl stearate)] using this method also resulted in uniform azimuthal alignment of 5CB, suggesting that the generation of long-range order in uniaxially compressed Langmuir films of polymers may also occur more generally over a broader range of polymers with flexible backbones.
doi:10.1016/j.jcis.2009.09.026
PMCID: PMC2785073  PMID: 19836025
Langmuir-Schaefer; Polymer; Liquid Crystals; Interfaces; Uniform Alignment
5.  Integration of Microsphere Resonators with Bioassay Fluidics for Whispering Gallery Mode Imaging 
The Analyst  2013;138(11):3189-3195.
Whispering gallery mode resonators are small, radially symmetric dielectrics that trap light through continuous total internal reflection. The resonant condition at which light is efficiently confined within the structure is linked with refractive index, which has led to the development of sensitive label-free sensing schemes based on whispering gallery mode resonators. One resonator design uses inexpensive high index glass microspheres that offer intrinsically superior optical characteristics, but have proven difficult to multiplex and integrate with the fluidics for sample delivery and fluid exchange necessary for assay development. Recently, we introduced a fluorescence imaging approach that enables large scale multiplexing with microsphere resonators, thus removing one obstacle for assay development. Here we report an approach for microsphere immobilization that overcomes limitations arising from their integration with fluidic delivery. The approach is an adaptation of a calcium-assisted glass bonding method originally developed for microfluidic glass chip fabrication. Microspheres bonded to glass using this technique are shown to be stable with respect to fluid flow and show no detectable loss in optical performance. Measured Q-factors, for example, remain unchanged following sphere bonding to the substrate. The stability of the immobilized resonators is further demonstrated by transferring lipid films onto the immobilized spheres using the Langmuir-Blodgett technique. Bilayers of DOPC doped with GM1 were transferred onto immobilized resonators to detect the binding of cholera toxin to GM1. Binding curves generated from shifts in the whispering gallery mode resonance result in a measured Kd of 1.5 × 10−11 with a limit of detection of 3.3 pM. These results are discussed in terms of future assay development using microsphere resonators.
doi:10.1039/c3an00328k
PMCID: PMC3734961  PMID: 23615457
6.  Aluminum Gallium Nitride (GaN)/GaN High Electron Mobility Transistor-Based Sensors for Glucose Detection in Exhaled Breath Condensate 
Background
Immobilized aluminum gallium nitride (AlGaN)/GaN high electron mobility transistors (HEMTs) have shown great potential in the areas of pH, chloride ion, and glucose detection in exhaled breath condensate (EBC). HEMT sensors can be integrated into a wireless data transmission system that allows for remote monitoring. This technology offers the possibility of using AlGaN/GaN HEMTs for extended investigations of airway pathology of detecting glucose in EBC without the need for clinical visits.
Methods
HEMT structures, consisting of a 3-μm-thick undoped GaN buffer, 30-Å-thick Al0.3Ga0.7N spacer, and 220-Å-thick silicon-doped Al0.3Ga0.7N cap layer, were used for fabricating the HEMT sensors. The gate area of the pH, chloride ion, and glucose detection was immobilized with scandium oxide (Sc2O3), silver chloride (AgCl) thin film, and zinc oxide (ZnO) nanorods, respectively.
Results
The Sc2O3-gated sensor could detect the pH of solutions ranging from 3 to 10 with a resolution of ∼0.1 pH. A chloride ion detection limit of 10-8 M was achievedt with a HEMT sensor immobilized with the AgCl thin film. The drain–source current of the ZnO nanorod-gated AlGaN/GaN HEMT sensor immobilized with glucose oxidase showed a rapid response of less than 5 seconds when the sensor was exposed to the target glucose in a buffer with a pH value of 7.4. The sensor could detect a wide range of concentrations from 0.5 nM to 125 μM.
Conclusion
There is great promise for using HEMT-based sensors to enhance the detection sensitivity for glucose detection in EBC. Depending on the immobilized material, HEMT-based sensors can be used for sensingt different materials. These electronic detection approaches with rapid response and good repeatability show potential for the investigation of airway pathology. The devices can also be integrated into a wireless data transmission system for remote monitoring applications. This sensor technology could use the exhaled breath condensate to measure the glucose concentration for diabetic applications.
PMCID: PMC2825639  PMID: 20167182
AlGaN/GaN; chloride ion; glucose; HEMT; noninvasive detection; pH; sensor
7.  Hydrogen Gas Sensors Based on Semiconductor Oxide Nanostructures 
Sensors (Basel, Switzerland)  2012;12(5):5517-5550.
Recently, the hydrogen gas sensing properties of semiconductor oxide (SMO) nanostructures have been widely investigated. In this article, we provide a comprehensive review of the research progress in the last five years concerning hydrogen gas sensors based on SMO thin film and one-dimensional (1D) nanostructures. The hydrogen sensing mechanism of SMO nanostructures and some critical issues are discussed. Doping, noble metal-decoration, heterojunctions and size reduction have been investigated and proved to be effective methods for improving the sensing performance of SMO thin films and 1D nanostructures. The effect on the hydrogen response of SMO thin films and 1D nanostructures of grain boundary and crystal orientation, as well as the sensor architecture, including electrode size and nanojunctions have also been studied. Finally, we also discuss some challenges for the future applications of SMO nanostructured hydrogen sensors.
doi:10.3390/s120505517
PMCID: PMC3386698  PMID: 22778599
hydrogen gas sensor; semiconductor oxides; nanostructure; thin films; one-dimensional nanostructures
8.  Emerging use of nanostructure films containing capped gold nanoparticles in biosensors 
The localized surface plasmon resonance (LSPR) property of gold nanoparticles (GNP) has been exploited in a variety of optical sensor configurations including solution-based bioassays, paper-based colorimetric detection, surface-confined nanoparticle film/array-based sensing, etc. Amongst these, gold nanostructured films are of great interest because of their high stability, good reproducibility, robustness, and cost-effectiveness. The inherent optical characteristics of GNP, are attributed to parameters like size and shape (eg, nanospheres, nanorods, nanostars), eg, LSPR spectral location sensitivity to the local environment, composition (eg, gold–silver or silica–gold nanoshells), sensing volume, mesospacing, and multiplexing. These properties allow sensor tunability, enabling enhanced sensitivity and better performance of these biosensors. Ultrasensitive biosensor designs were realized using gold nanostructured films fabricated by bottom-up as well as top-down approaches. In this review, we describe the past, present, and future trends in the development of GNP-LSPR-based sensors, concentrating on both design (fabrication) and application. In the process, we have discussed various combinations of GNP size and shape, substrate, and application domains.
doi:10.2147/NSA.S8981
PMCID: PMC3781700  PMID: 24198481
localized surface plasmon resonance; gold nanoparticles; label-free optical biosensor
9.  Comparative Study of Alternating Low-band-Gap Benzothiadiazole Co-oligomers 
Journal of Fluorescence  2011;21(4):1625-1633.
The benzothiadiazole – arylene alternating conjugated oligomers have been designed and synthesized via Suzuki coupling reaction. The structures and properties of the conjugated oligomers were characterized by 1HNMR, 13CNMR, UV–vis absorption spectroscopy, photoluminescence (PL) spectroscopy. The luminescent measurements demonstrate that polybenzothiadiazoles are good chromophores able to form thin films by Langmuir-Blodgett (LB) technique, making them suitable for further applications. Also the electrical properties of obtained films confirm the good potential of these novel aryl-based π-conjugated polymers for the development of various electrical and electrochemical solid-state devices.
doi:10.1007/s10895-011-0851-1
PMCID: PMC3144376  PMID: 21279539
Benzothiadiazole; Copolymers; Suzuki coupling; Electroconductivity; Luminescence; Atomic force microscopy
10.  Formation of net-like patterns of gold nanoparticles in liquid crystal matrix at the air–water interface 
Controlled patterning and formation of nanostructures on surfaces based on self-assembly is a promising area in the field of “bottom-up” nanomaterial engineering. We report formation of net-like structures of gold nanoparticles (Au NPs) in a matrix of liquid crystalline amphiphile 4′-n-octyl-4-cyanobiphenyl at the air–water interface. After initial compression to at least 18 mN m−1, decompression of a Langmuir film of a mixture containing both components results in formation of net-like structures. The average size of a unit cell of the net is easily adjustable by changing the surface pressure during the decompression of the film. The net-like patterns of different, desired average unit cell areas were transferred onto solid substrates (Langmuir–Blodgett method) and investigated with scanning electron microscopy and X-ray reflectivity (XRR). Uniform coverage over large areas was proved. XRR data revealed lifting of the Au NPs from the surface during the formation of the film. A molecular mechanism of formation of the net-like structures is discussed.
Electronic supplementary material
The online version of this article (doi:10.1007/s11051-012-0826-4) contains supplementary material, which is available to authorized users.
doi:10.1007/s11051-012-0826-4
PMCID: PMC3394235  PMID: 22798726
Gold nanoparticles; Langmuir films; Langmuir–Blodgett films; Nanostructures; Net; Nanoporosity
11.  Characterization of a novel ultra low refractive index material for biosensor application 
Sensors and actuators. B, Chemical  2009;141(1):227-232.
Nanoporous materials can provide significant benefits to the field of biosensors. Their size and porous structure makes them an ideal tool for improving sensor performance. This study characterized a novel ultra low index of refraction nanoporous organosilicate (NPO) material for use as an optical platform for fluorescence-based optical biosensors. While serving as the low index cladding material, the novel coating based on organosilicate nanoparticles also provides an opportunity for a high surface area coating that can be utilized for immobilizing biological probes. Biological molecules were immobilized onto NPO, which was spin-coated on silicon and glass substrates. The biological molecule was composed of Protein A conjugated to AlexaFluor 546 fluorophore and then immobilized onto the NPO substrate via silanization. Sample analysis consisted of spectrofluorometry, FT-IR spectroscopy, scanning electron microscopy, contact angle measurement and ellipsometry. The results showed the presence of emission peaks at 574 nm, indicating that the immobilization of Protein A to the NPO material is possible. When compared to Si and glass substrates not coated with NPO, the results showed a 100X and 10X increase in packing density with the NPO coated films respectively. Ellipsometric analysis, FT-IR, contact angle, and SEM imaging of the surface immobilized NPO films suggested that while the surface modifications did induce some damage, it did not incur significant changes to its unique characteristics, i.e., pore structure, wettability and index of refraction. It was concluded that NPO films would be a viable sensor substrate to enhance sensitivity and improve sensor performance.
doi:10.1016/j.snb.2009.04.034
PMCID: PMC2734105  PMID: 20161155
nanoporous material; biosensor; protein immobilization
12.  Fast-Response, Sensitivitive and Low-Powered Chemosensors by Fusing Nanostructured Porous Thin Film and IDEs-Microheater Chip 
Scientific Reports  2013;3:1669.
The chemiresistive thin film gas sensors with fast response, high sensitivity, low power consumption and mass-produced potency, have been expected for practical application. It requires both sensitive materials, especially exquisite nanomaterials, and efficient substrate chip for heating and electrical addressing. However, it is challenging to achieve repeatable microstructures across the films and low power consumption of substrate chip. Here we presented a new sensor structure via the fusion of metal-oxide nanoporous films and micro-electro-mechanical systems (MEMS)-based sensing chip. An interdigital-electrodes (IDEs) and microheater integrated MEMS structure is designed and employed as substrate chip to in-situ fabricate colloidal monolayer template-induced metal-oxide (egg. SnO2) nanoporous sensing films. This fused sensor demonstrates mW-level low power, ultrafast response (~1 s), and parts-per-billion lever detection for ethanol gas. Due to the controllable template strategy and mass-production potential, such micro/nano fused high-performance gas sensors will be next-generation key miniaturized/integrated devices for advanced practical applications.
doi:10.1038/srep01669
PMCID: PMC3628220  PMID: 23591580
13.  A non-labeled DNA biosensor based on light addressable potentiometric sensor modified with TiO2 thin film*  
Titanium dioxide (TiO2) thin film was deposited on the surface of the light addressable potentiometric sensor (LAPS) to modify the sensor surface for the non-labeled detection of DNA molecules. To evaluate the effect of ultraviolet (UV) treatment on the silanization level of TiO2 thin film by 3-aminopropyltriethoxysilane (APTS), fluorescein isothiocyanate (FITC) was used to label the amine group on the end of APTS immobilized onto the TiO2 thin film. We found that, with UV irradiation, the silanization level of the irradiated area of the TiO2 film was improved compared with the non-irradiated area under well-controlled conditions. This result indicates that TiO2 can act as a coating material on the biosensor surface to improve the effect and efficiency of the covalent immobilization of biomolecules on the sensor surface. The artificially synthesized probe DNA molecules were covalently linked onto the surface of TiO2 film. The hybridization of probe DNA and target DNA was monitored by the recording of I-V curves that shift along the voltage axis during the process of reaction. A significant LAPS signal can be detected at 10 μmol/L of target DNA sample.
doi:10.1631/jzus.B0920090
PMCID: PMC2772892  PMID: 19882762
DNA biosensor; Titanium dioxide (TiO2) thin film; Light addressable potentiometric sensor (LAPS); Silanization; Fluorescein label; Gene chip
14.  Metal Oxide Nanostructures and Their Gas Sensing Properties: A Review 
Sensors (Basel, Switzerland)  2012;12(3):2610-2631.
Metal oxide gas sensors are predominant solid-state gas detecting devices for domestic, commercial and industrial applications, which have many advantages such as low cost, easy production, and compact size. However, the performance of such sensors is significantly influenced by the morphology and structure of sensing materials, resulting in a great obstacle for gas sensors based on bulk materials or dense films to achieve highly-sensitive properties. Lots of metal oxide nanostructures have been developed to improve the gas sensing properties such as sensitivity, selectivity, response speed, and so on. Here, we provide a brief overview of metal oxide nanostructures and their gas sensing properties from the aspects of particle size, morphology and doping. When the particle size of metal oxide is close to or less than double thickness of the space-charge layer, the sensitivity of the sensor will increase remarkably, which would be called “small size effect”, yet small size of metal oxide nanoparticles will be compactly sintered together during the film coating process which is disadvantage for gas diffusion in them. In view of those reasons, nanostructures with many kinds of shapes such as porous nanotubes, porous nanospheres and so on have been investigated, that not only possessed large surface area and relatively mass reactive sites, but also formed relatively loose film structures which is an advantage for gas diffusion. Besides, doping is also an effective method to decrease particle size and improve gas sensing properties. Therefore, the gas sensing properties of metal oxide nanostructures assembled by nanoparticles are reviewed in this article. The effect of doping is also summarized and finally the perspectives of metal oxide gas sensor are given.
doi:10.3390/s120302610
PMCID: PMC3376589  PMID: 22736968
metal oxide; gas sensing; nanostructure; size effect; doping
15.  Biomedical Detection via Macro- and Nano-Sensors Fabricated with Metallic and Semiconducting Oxides 
Originally developed as gas sensors, the benefits of metallic and semiconducting oxide materials are now being realized in other areas of sensing, such as chemical, environmental, and biomedical monitoring and detection. Metallic and semiconducting oxides have continuously expanded their roles to date, and have also established their significance in biosensing by utilizing a variety of modes for signal generation and detection mechanism. These sensors are typically based either on their optical, electrochemical, electrical, gravimetric, acoustic, and magnetic properties for signal transduction. This article reviews such biosensors that employ metallic and semiconducting oxides as active sensing elements to detect nucleic acids, proteins, cells, and a variety of important biomarkers, both in thin film and one-dimensional forms. Specific oxide materials (Mx Oy ) examined comprehensively in this article include M = Fe, Cu, Si, Zn, Sn, In. The derivatives of these oxide materials resulting from incorporation of dopants are examined as well. The crystalline structures and unique properties that may be exploited for various biosensing applications are discussed, and recent efforts investigating the feasibility of using these oxide materials in biosensor technology are described. Key biosensor characteristics resulting from reduced dimensionality are overviewed under the motif of planar and one-dimensional sensors. This article also provides insight into current challenges facing biosensor applications for metallic and semiconducting oxides. In addition, future outlook in this particular field as well as different impacts on biology and medicine are addressed.
PMCID: PMC3766318  PMID: 23627064
Semiconducting Oxides; Metallic Oxides; Biosensors; Solid-State Biodetection; Nanobiosensors; Nanomaterials; Biomedical Detection
16.  A Dry Membrane Protection Technique to Allow Surface Acoustic Wave Biosensor Measurements of Biological Model Membrane Approaches 
Sensors (Basel, Switzerland)  2013;13(9):12392-12405.
Model membrane approaches have attracted much attention in biomedical sciences to investigate and simulate biological processes. The application of model membrane systems for biosensor measurements is partly restricted by the fact that the integrity of membranes critically depends on the maintenance of an aqueous surrounding, while various biosensors require a preconditioning of dry sensors. This is for example true for the well-established surface acoustic wave (SAW) biosensor SAM®5 blue. Here, a simple drying procedure of sensor-supported model membranes is introduced using the protective disaccharide trehalose. Highly reproducible model membranes were prepared by the Langmuir-Blodgett technique, transferred to SAW sensors and supplemented with a trehalose solution. Membrane rehydration after dry incorporation into the SAW device becomes immediately evident by phase changes. Reconstituted model membranes maintain their full functionality, as indicated by biotin/avidin binding experiments. Atomic force microscopy confirmed the morphological invariability of dried and rehydrated membranes. Approximating to more physiological recognition phenomena, the site-directed immobilization of the integrin VLA-4 into the reconstituted model membrane and subsequent VCAM-1 ligand binding with nanomolar affinity were illustrated. This simple drying procedure is a novel way to combine the model membrane generation by Langmuir-Blodgett technique with SAW biosensor measurements, which extends the applicability of SAM®5 blue in biomedical sciences.
doi:10.3390/s130912392
PMCID: PMC3821348  PMID: 24064603
biosensor; Langmuir-Blodgett technique; membrane protection; SAW; trehalose
17.  Zeolite-based Impedimetric Gas Sensor Device in Low-cost Technology for Hydrocarbon Gas Detection 
Sensors (Basel, Switzerland)  2008;8(12):7904-7916.
Due to increasing environmental concerns the need for inexpensive selective gas sensors is increasing. This work deals with transferring a novel zeolite-based impedimetric hydrocarbon gas sensor principle, which has been originally manufactured in a costly combination of photolithography, thin-film processes, and thick-film processes to a low-cost technology comprising only thick-film processes and one electroplating step. The sensing effect is based on a thin chromium oxide layer between the interdigital electrodes and a Pt-loaded ZSM-5 zeolite film. When hydrocarbons are present in the sensor ambient, the electrical sensor impedance increases strongly and selectively. In the present work, the chromium oxide film is electroplated on Au screen-printed interdigital electrodes and then oxidized to Cr2O3. The electrode area is covered with the screen-printed zeolite. The sensor device is self-heated utilizing a planar platinum heater on the backside. The best sensor performance is obtained at a frequency of 3 Hz at around 350 °C. The good selectivity of the original sensor setup could be confirmed, but a strong cross-sensitivity to ammonia occurs, which might prohibit its original intention for use in automotive exhausts.
doi:10.3390/s8127904
PMCID: PMC3790997
OBD (On-Board-Diagnosis); electroplating; HC; VOC
18.  Cell-directed-assembly: Directing the formation of nano/bio interfaces and architectures with living cells 
Biochimica et biophysica acta  2010;1810(3):259-267.
Background
The desire to immobilize, encapsulate, or entrap viable cells for use in a variety of applications has been explored for decades. Traditionally, the approach is to immobilize cells to utilize a specific functionality of the cell in the system.
Scope of Review
This review describes our recent discovery that living cells can organize extended nanostructures and nano-objects to create a highly biocompatible nano//bio interface [1].
Major Conclusions
We find that short chain phospholipids direct the formation of thin film silica mesophases during evaporation-induced self-assembly (EISA) [2], and that the introduction of cells alter the self-assembly pathway. Cells organize an ordered lipid-membrane that forms a coherent interface with the silica mesophase that is unique in that it withstands drying - yet it maintains accessibility to molecules introduced into the 3D silica host. Cell viability is preserved in the absence of buffer, making these constructs useful as standalone cell-based sensors. In response to hyperosmotic stress, the cells release water, creating a pH gradient which is maintained within the nanostructured host and serves to localize lipids, proteins, plasmids, lipidized nanocrystals, and other components at the cellular surface. This active organization of the bio/nano interface can be accomplished during ink-jet printing or selective wetting - processes allowing patterning of cellular arrays - and even spatially-defined genetic modification.
General Significance
Recent advances in the understanding of nanotechnology and cell biology encourage the pursuit of more complex endeavors where the dynamic interactions of the cell and host material act symbiotically to obtain new, useful functions.
doi:10.1016/j.bbagen.2010.09.005
PMCID: PMC3090153  PMID: 20933574
19.  Self-activated ultrahigh chemosensitivity of oxide thin film nanostructures for transparent sensors 
Scientific Reports  2012;2:588.
One of the top design priorities for semiconductor chemical sensors is developing simple, low-cost, sensitive and reliable sensors to be built in handheld devices. However, the need to implement heating elements in sensor devices, and the resulting high power consumption, remains a major obstacle for the realization of miniaturized and integrated chemoresistive thin film sensors based on metal oxides. Here we demonstrate structurally simple but extremely efficient all oxide chemoresistive sensors with ~90% transmittance at visible wavelengths. Highly effective self-activation in anisotropically self-assembled nanocolumnar tungsten oxide thin films on glass substrate with indium-tin oxide electrodes enables ultrahigh response to nitrogen dioxide and volatile organic compounds with detection limits down to parts per trillion levels and power consumption less than 0.2 microwatts. Beyond the sensing performance, high transparency at visible wavelengths creates opportunities for their use in transparent electronic circuitry and optoelectronic devices with avenues for further functional convergence.
doi:10.1038/srep00588
PMCID: PMC3421433  PMID: 22905319
20.  Formation of protein molecular imprints within Langmuir monolayers: A quartz crystal microbalance study 
Protein imprinting leading to enhanced rebinding of ferritin to ternary lipid monolayers is demonstrated using a quartz crystal microbalance. Monolayers consisting of cationic dioctadecyldimethylammonium bromide, non-ionic methyl stearate, and poly(ethylene glycol) bearing phospholipids were imprinted with ferritin at the air/water interface of a Langmuir-Blodgett trough and transferred hydrated to hydrophobic substrates for study. This immobilization was shown by fluorescence correlation spectroscopy to significantly hinder any further diffusion of lipids, while rebinding studies demonstrated up to a six-fold increase in ferritin adsorption to imprinted versus control monolayers. A diminished rebinding of ferritin to its imprint was observed through pH reduction to below the protein isoelectric point, demonstrating the electrostatic nature of the interaction. Rebinding to films where imprint pockets remained occupied by the template protein was also minimal. Studies with a smaller acidic protein revealed the importance of the steric influence of poly(ethylene glycol) in forming the protein binding pockets, as albumin-imprinted monolayers showed low binding of ferritin, while ferritin-imprinted monolayers readily accommodated albumin. The controllable structure-function relationship and limitations of this system are discussed with respect to the application of protein imprinting in sensor development as well as fundamental studies of proteins at dynamic interfaces.
doi:10.1016/j.jcis.2006.12.037
PMCID: PMC2632306  PMID: 17204279
Protein adsorption; Molecular imprinting; Langmuir monolayer; Mixed monolayer; Quartz crystal microbalance; QCM; Fluorescence correlation spectroscopy; FCS; Poly(ethylene glycol); PEG; Ferritin
21.  Pd Nanoparticles and Thin Films for Room Temperature Hydrogen Sensor 
Nanoscale Research Letters  2009;4(10):1191-1196.
We report the application of palladium nanoparticles and thin films for hydrogen sensor. Electrochemically grown palladium particles with spherical shapes deposited on Si substrate and sputter deposited Pd thin films were used to detect hydrogen at room temperature. Grain size dependence of H2 sensing behavior has been discussed for both types of Pd films. The electrochemically grown Pd nanoparticles were observed to show better hydrogen sensing response than the sputtered palladium thin films. The demonstration of size dependent room temperature H2 sensing paves the ways to fabricate the room temperature metallic and metal–metal oxide semiconductor sensor by tuning the size of metal catalyst in mixed systems. H2 sensing by the Pd nanostructures is attributed to the chemical and electronic sensitization mechanisms.
doi:10.1007/s11671-009-9379-6
PMCID: PMC2894097  PMID: 20596429
Palladium; Hydrogen sensors
22.  Pd Nanoparticles and Thin Films for Room Temperature Hydrogen Sensor 
Nanoscale Research Letters  2009;4(10):1191-1196.
We report the application of palladium nanoparticles and thin films for hydrogen sensor. Electrochemically grown palladium particles with spherical shapes deposited on Si substrate and sputter deposited Pd thin films were used to detect hydrogen at room temperature. Grain size dependence of H2sensing behavior has been discussed for both types of Pd films. The electrochemically grown Pd nanoparticles were observed to show better hydrogen sensing response than the sputtered palladium thin films. The demonstration of size dependent room temperature H2sensing paves the ways to fabricate the room temperature metallic and metal–metal oxide semiconductor sensor by tuning the size of metal catalyst in mixed systems. H2sensing by the Pd nanostructures is attributed to the chemical and electronic sensitization mechanisms.
doi:10.1007/s11671-009-9379-6
PMCID: PMC2894097  PMID: 20596429
Palladium; Hydrogen sensors
23.  Acoustoelectric Effect on the Responses of SAW Sensors Coated with Electrospun ZnO Nanostructured Thin Film 
Sensors (Basel, Switzerland)  2012;12(9):12006-12015.
In this study, zinc oxide (ZnO) was a very good candidate for improving the sensitivity of gas sensor technology. The preparation of an electrospun ZnO nanostructured thin film on a 433 MHz Rayleigh wave based Surface Acoustic Wave (SAW) sensor and the investigation of the acoustoelectric effect on the responses of the SAW sensor are reported. We prepared an electrospun ZnO nanostructured thin film on the SAW devices by using an electrospray technique. To investigate the dependency of the sensor response on the structure and the number of the ZnO nanoparticles, SAW sensors were prepared with different coating loads. The coating frequency shifts were adjusted to fall between 100 kHz and 2.4 MHz. The sensor measurements were performed against VOCs such as acetone, trichloroethylene, chloroform, ethanol, n-propanol and methanol vapor. The sensor responses of n-propanol have opposite characteristics to the other VOCs, and we attributed these characteristics to the elastic effect/acoustoelectric effect.
doi:10.3390/s120912006
PMCID: PMC3478823
surface acoustic waves; zinc oxide; nanostructures; electrospun; acoustoelectric effect
24.  A Conductometric Indium Oxide Semiconducting Nanoparticle Enzymatic Biosensor Array 
Sensors (Basel, Switzerland)  2011;11(10):9300-9312.
We report a conductometric nanoparticle biosensor array to address the significant variation of electrical property in nanomaterial biosensors due to the random network nature of nanoparticle thin-film. Indium oxide and silica nanoparticles (SNP) are assembled selectively on the multi-site channel area of the resistors using layer-by-layer self-assembly. To demonstrate enzymatic biosensing capability, glucose oxidase is immobilized on the SNP layer for glucose detection. The packaged sensor chip onto a ceramic pin grid array is tested using syringe pump driven feed and multi-channel I–V measurement system. It is successfully demonstrated that glucose is detected in many different sensing sites within a chip, leading to concentration dependent currents. The sensitivity has been found to be dependent on the channel length of the resistor, 4–12 nA/mM for channel lengths of 5–20 μm, while the apparent Michaelis-Menten constant is 20 mM. By using sensor array, analytical data could be obtained with a single step of sample solution feeding. This work sheds light on the applicability of the developed nanoparticle microsensor array to multi-analyte sensors, novel bioassay platforms, and sensing components in a lab-on-a-chip.
doi:10.3390/s111009300
PMCID: PMC3231260  PMID: 22163696
biosensor array; nanoparticle; conductometric sensor; microsensor array; glucose sensor
25.  Contact CMOS imaging of gaseous oxygen sensor array 
We describe a compact luminescent gaseous oxygen (O2) sensor microsystem based on the direct integration of sensor elements with a polymeric optical filter and placed on a low power complementary metal-oxide semiconductor (CMOS) imager integrated circuit (IC). The sensor operates on the measurement of excited-state emission intensity of O2-sensitive luminophore molecules tris(4,7-diphenyl-1,10-phenanthroline) ruthenium(II) ([Ru(dpp)3]2+) encapsulated within sol–gel derived xerogel thin films. The polymeric optical filter is made with polydimethylsiloxane (PDMS) that is mixed with a dye (Sudan-II). The PDMS membrane surface is molded to incorporate arrays of trapezoidal microstructures that serve to focus the optical sensor signals on to the imager pixels. The molded PDMS membrane is then attached with the PDMS color filter. The xerogel sensor arrays are contact printed on top of the PDMS trapezoidal lens-like microstructures. The CMOS imager uses a 32 × 32 (1024 elements) array of active pixel sensors and each pixel includes a high-gain phototransistor to convert the detected optical signals into electrical currents. Correlated double sampling circuit, pixel address, digital control and signal integration circuits are also implemented on-chip. The CMOS imager data is read out as a serial coded signal. The CMOS imager consumes a static power of 320 µW and an average dynamic power of 625 µW when operating at 100 Hz sampling frequency and 1.8 V DC. This CMOS sensor system provides a useful platform for the development of miniaturized optical chemical gas sensors.
doi:10.1016/j.snb.2011.04.074
PMCID: PMC3909528  PMID: 24493909
Contact imaging; CMOS imager; Xerogel thin-films; Gas sensors; O2 sensors; Optical sensors; Luminescence; PDMS; Microlens

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