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Little has been studied on how the electrochemical noise impacts the limit of detection of field effect transistor (FET) biosensors. Herein, we investigate low frequency noise associated with phosphate-buffered saline (PBS) solutions at varying ionic strengths (Ni) under both weak and strong gate biases corresponding to saturation and sub-threshold regimes, respectively, in AlGaN/GaN heterojunction FET biosensors. We show that the electrochemical noise is strongly dependent on the ionic strength and gate biasing conditions. In the saturation regime (low bias), varying the ionic strength (a range of 10−6× PBS to PBS 1 × stock solutions used for testing) has little to no effect on the characteristic frequency exponent 𝛽(𝛽=1), indicating a predominately diffusion-based process. Conversely, under higher biases (sub-threshold regime), the β parameter varies from 1 to 2 with ionic strength exhibiting both diffusion and drift characteristics, with a “cut point” at approximately 10−5× PBS (𝑁𝑖≈9×1014/mL). Under a high bias, once the PBS concentration reaches 10−3×, the behavior is then drift dominant. This indicates that the higher bias likely triggers electrochemical reactions and by extension, faradaic effects at most physiologically relevant ionic strengths. The signal-to-noise ratio (SNR) of the device has an inverse linear relationship with the low frequency current noise. The device exhibits a higher SNR in the sub-threshold regime than in the saturation regime. Specifically, within the saturation regime, an inversely proportional relationship between the SNR and the ionic concentration is observed. The electrochemical noise induced from ionic activities is roughly proportional to 𝑁−1/2𝑖.
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Optimization of Electrolytes with Redox Reagents to Improve the Impedimetric Signal for Use with a Low-Cost Analyzer
The most well-known criterion for POC devices is ASSURED, and affordability, i.e., using low-cost instrumentation, is the most challenging one. This manuscript provides a pathway for transitioning ESSENCE, an impedance-based biosensor platform, from using an expensive benchtop analyzer—KeySight 4294A (~$50k)—to using a significantly portable and cheaper USB oscilloscope—Analog Discovery 2 (~$200) —with similar sensitivity (around 100 times price difference). To achieve this, we carried out a fundamental study of the interplay between an electrolyte like potassium chloride (KCl), and an electrolyte buffer like phosphate buffered saline (PBS) in the presence and absence of a redox buffer like ferro/ferricyanide system and ([Ru(bpy)3]2+). Redox molecules in the electrolyte caused a significant change in the Nyquist curve of the impedance depending on the redox molecule type. The redox species and the background electrolyte have their own RC semicircles in the Nyquist curve, whose overlap depends on the redox concentration and electrolyte ionic strength. We found that by increasing the electrolyte ionic strength or the redox concentration, the RC semicircle moves to higher frequencies and vice versa. Importantly, the use of the buffer electrolyte, instead of KCl, led to a lower standard deviation and overall signal (lesser sensitivity). However, to achieve the best results from the biorecognition signal, we chose a buffered electrolyte like PBS with high ionic strength and lowered the redox probe concentrations to minimize the standard deviation and reduce any noise from migrating to the low-cost analyzer. Comparing the two analyzers shows similar results, with a lowered detection limit from the low-cost analyzer.
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- Award ID(s):
- 1751759
- PAR ID:
- 10565806
- Publisher / Repository:
- Biosensor
- Date Published:
- Journal Name:
- Biosensors
- Volume:
- 13
- Issue:
- 12
- ISSN:
- 2079-6374
- Page Range / eLocation ID:
- 999
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.3390/bios13120999
