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This article describes the fabrication, characterization and application of an epidermal temporary-transfer tattoo-based potentiometric sensor, coupled with a miniaturized wearable wireless transceiver, for real-time monitoring of sodium in the human perspiration. Sodium excreted during perspiration is an excellent marker for electrolyte imbalance and provides valuable information regarding an individual's physical and mental wellbeing. The realization of the new skin-worn non-invasive tattoo-like sensing device has been realized by amalgamating several state-of-the-art thick film, laser printing, solid-state potentiometry, fluidics and wireless technologies. The resulting tattoo-based potentiometric sodium sensor displays a rapid near-Nernstian response with negligible carryover effects, and good resiliency against various mechanical deformations experienced by the human epidermis. On-body testing of the tattoo sensor coupled to a wireless transceiver during exercise activity demonstrated its ability to continuously monitor sweat sodium dynamics. The real-time sweat sodium concentration was transmitted wirelessly via a body-worn transceiver from the sodium tattoo sensor to a notebook while the subjects perspired on a stationary cycle. The favorable analytical performance along with the wearable nature of the wireless transceiver makes the new epidermal potentiometric sensing system attractive for continuous monitoring the sodium dynamics in human perspiration during diverse activities relevant to the healthcare, fitness, military, healthcare and skin-care domains.
Light-addressable potentiometric sensors (LAPS) consisting of a p-Si-SiO2 and p-Si-SiO2-Au structure, respectively, have been tested for a label-free electrical detection of DNA (deoxyribonucleic acid) hybridization. Three different strategies for immobilizing single-stranded probe DNA (ssDNA) molecules on a LAPS surface have been studied and compared: (a) immobilization of thiol-modified ssDNA on the patterned Au surface via gold-thiol bond, (b) covalent immobilization of amino-modified ssDNA onto the SiO2 surface functionalized with 3-aminopropyltriethoxysilane and (c) layer-by-layer adsorption of negatively charged ssDNA on a positively charged weak polyelectrolyte layer of poly(allylamine hydrochloride).
Planar and three-dimensional (3D) interdigitated electrodes (IDE) with electrode digits separated by an insulating barrier of different heights were electrochemically characterized and compared in terms of their sensing properties. Due to the impact of the surface resistance, both types of IDE structures display a non-linear behavior in low-ionic strength solutions. The experimental data were fitted to an electrical equivalent circuit and interpreted taking into account the surface-charge-governed properties. The effect of a charged polyelectrolyte layer electrostatically assembled onto the sensor surface on the surface resistance in solutions with different KCl concentration is studied. In case of the same electrode footprint, 3D-IDEs show a larger cell constant and a higher sensitivity to molecular adsorption than that of planar IDEs. The obtained results demonstrate the potential of 3D-IDEs as a new transducer structure for a direct label-free sensing of charged molecules.
The light-addressable potentiometric sensor (LAPS) is a semiconductor-based potentiometric sensor using a light probe with an ability of detecting the concentration of biochemical species in a spatially resolved manner. As an important biomedical sensor, research has been conducted to improve its performance, for instance, to realize high-speed measurement. In this work, the idea of facilitating the device-level simulation, instead of using an equivalent-circuit model, is presented for detailed analysis and optimization of the performance of the LAPS. Both carrier distribution and photocurrent response have been simulated to provide new insight into both amplitude-mode and phase-mode operations of the LAPS. Various device parameters can be examined to effectively design and optimize the LAPS structures and setups for enhanced performance.
As a semiconductor-based electrochemical sensor, the light-addressable potentiometric sensor (LAPS) can realize two dimensional visualization of (bio-)chemical reactions at the sensor surface addressed by localized illumination. Thanks to this imaging capability, various applications in biochemical and biomedical fields are expected, for which the spatial resolution is critically significant. In this study, therefore, the spatial resolution of the LAPS was investigated in detail based on the device simulation. By calculating the spatiotemporal change of the distributions of electrons and holes inside the semiconductor layer in response to a modulated illumination, the photocurrent response as well as the spatial resolution was obtained as a function of various parameters such as the thickness of the Si substrate, the doping concentration, the wavelength and the intensity of illumination.
The simulation results verified that both thinning the semiconductor substrate and increasing the doping concentration could improve the spatial resolution, which were in good agreement with known experimental results and theoretical analysis. More importantly, new findings of interests were also obtained. As for the dependence on the wavelength of illumination, it was found that the known dependence was not always the case. When the Si substrate was thick, a longer wavelength resulted in a higher spatial resolution which was known by experiments. When the Si substrate was thin, however, a longer wavelength of light resulted in a lower spatial resolution. This finding was explained as an effect of raised concentration of carriers, which reduced the thickness of the space charge region.
The device simulation was found to be helpful to understand the relationship between the spatial resolution and device parameters, to understand the physics behind it, and to optimize the device structure and measurement conditions for realizing higher performance of chemical imaging systems.
A novel photoexcitation method for the light-addressable potentiometric sensor (LAPS) is proposed to achieve a higher spatial resolution of chemical images. The proposed method employs a combined light source that consists of a modulated light probe, which generates the alternating photocurrent signal, and a ring of constant illumination surrounding it. The constant illumination generates a sheath of carriers with increased concentration which suppresses the spread of photocarriers by enhanced recombination. A device simulation was carried out to verify the effect of constant illumination on the spatial resolution, which demonstrated that a higher spatial resolution can be obtained.
A novel photoexcitation method for the light-addressable potentiometric sensor (LAPS) realized a higher spatial resolution of chemical imaging. In this method, a modulated light probe, which generates the alternating photocurrent signal, is surrounded by a ring of constant light, which suppresses the lateral diffusion of photocarriers by enhancing recombination. A device simulation verified that a higher spatial resolution could be obtained by adjusting the gap between the modulated and constant light. It was also found that a higher intensity and a longer wavelength of constant light was more effective. However, there exists a tradeoff between the spatial resolution and the amplitude of the photocurrent, and thus, the signal-to-noise ratio. A tilted incidence of constant light was applied, which could achieve even higher resolution with a smaller loss of photocurrent.