Fluorometric detection of sulfate-reducing bacteria via the aggregation-induced emission of glutathione-gold(I) complexes.

It is reported that gold(I)-thiolate complexes can display aggregation-induced emission (AIE) similar to organic fluorogens. On addition of lead(II) to glutathione-gold(I) complexes, a supermolecular structure of type GSH-Au(I)-Pb(II) is formed through strong coordination between Pb(II) and GSH. Its fluorescence is quenched by sulfide due to the formation of PbS which destroys the GSH-Au(I)-Pb(II) complex. The finding was used to design a method for fluorometric detection of sulfate-reducing bacteria (SRB) which produce sulfide. The time needed to reduce fluorescence to 10% of its initial intensity linearly dependent on the logarithm of the SRB concentrations in the ranging from 10 to 1 × 10^7 cfu mL-1. The assay time is also reduced down to 4 days even if the SRB concentration is as low as 10 cfu mL-1. Graphical abstract Schematic presentation of aggregation-induced emission (AIE)-active GSH-Au(I) complexes based fluorescence detection of SRB. The GSH-Au(I) complexes turn into aggregation and display strong emissive property in the presence of Pb2+. Then the fluorescence of GSH-Au(I)-Pb(II) complexes can be quenched by S2- generated by SRB.

Cost-Effective Nanophotonic Metasurfaces with Spatially Gradient Structures for Ultrasensitive Imaging-Based Refractometric Sensing.

Nanophotonic metasurfaces are widely utilized in various domains, such as biomedical, healthcare, and environmental monitoring, benefiting from their unique advantages of label-free, noninvasive, and real-time response. However, nanophotonic metasurfaces usually rely on sophisticated instruments, and expensive and time-consuming fabrication processes, which severely restricts their practical applications. Herein, a spatially gradient metasurface is integrated with an imaging-based sensing scheme, waiving the requirement of spectrometers and achieving an ultrahigh imaging-based sensitivity of 3321 pixels/refractive index unit superior to that characterized using conventional compact spectrometers. The metasurface is fabricated by nanoimprint lithography using a reusable cyclic olefin copolymer template featuring millions of unique nanostructures. Under the illumination of monochromatic light, the transmittance of different nanostructures on the metasurface differs, resulting in grayscale images with varied intensity distributions. Analyzing the intensity change of the metasurface's recorded image can obtain the covering medium's refractive index. Furthermore, through theory and experimentation, the high reliability of the proposed reusable and flexible template has been verified for nanophotonic metasurface fabrication which further reduces the fabrication cost of core sensing elements. Finally, with proper optimization of the metasurface structure and imaging system, this setup is expected to be applied to many emerging areas of point-of-care, real-time, and on-site biosensing.

Multi-biomarker combination detection system for diagnosis and classification of dry eye disease by imaging of a multi-channel metasurface.

Dry eye disease (DED) is one of the most common ocular surface diseases, characterized by unstable tear film and ocular inflammation, affecting hundreds of millions of people worldwide. Currently, the clinical diagnosis of DED mainly relies on physical methods such as optical microscopy and ocular surface interferometric imaging, but classifying DED is still difficult. Here, we propose a compact and portable immune detection system based on the direct imaging of a nanophotonic metasurface with gradient geometry, for fast and ultra-sensitive detection of multiple biomarkers (i.e. Matrix metalloproteinase-9 (MMP-9), Lipocalin-1 (LCN-1), Lactoferrin (LTF)) in tears for the diagnosis and classification of DED. This centimeter-scale concentric nanophotonic metasurface, which consists of millions of unique metallic nanostructures, was fabricated through a cost-effective nanoimprint lithography (NIL) process. The immune detection system based on the antibody-modified metasurface shows favorable detection selectivity, an ultra-high sensitivity (3350 pixels/Refractive Index Unit (RIU)) and low limit of detection (LOD) (0.3 ng/mL for MMP-9, 1 ng/mL for LTF, and 0.5 ng/mL for LCN-1). Further clinical sampling and detection results demonstrated that this multi-biomarker detection system enabled accurate determination and symptom classification of DED, manifesting high correlation and consistency with clinical diagnosis results. The advantages such as low sample consumption, one-step detection, simple operation, and simultaneous detection of multiple biomarkers make the platform promising for screening and detecting a broader range of biomarker combinations in clinical practice.

Facile fabrication of highly sensitive and non-label aptasensors based on antifouling amyloid-like protein aggregates.

In this paper, we present a robust and versatile method for developing non-label aptasensors with high sensitivity. Amyloid-like protein aggregates were facilely synthesized with the commonly used passivating agent bovine serum albumin (BSA) in developing biosensors, and the produced amyloid-like phase-transited BSA (PTB) exhibited excellent antifouling performances and robust interfacial adhesion with the electrode surface. In order to improve the detection sensitivity of electrochemical measurements, reduced graphene oxide was electrochemically deposited onto the electrode surface. Moreover, gold nanoparticles were introduced to enhance the conductivity of the PTB film and facilitate subsequent aptamer modification. Two common biological species, adenosine triphosphate (ATP) and cytochrome c (cyt c), were chosen as detection targets, and their corresponding aptasensors were successfully constructed and systematically evaluated. The proposed aptasensors based on the PTB-Au antifouling composite exhibited high sensitivity and specificity towards ATP and cyt c detection, and the detection limits were calculated to be 0.26 nM and 0.64 nM for ATP and cyt c, respectively. Hence, this work provides a simple approach to develop highly sensitive aptasensors without any labeling process, and thus promises its great application in biological analysis.

Ultrasensitive Molecular Detection at Subpicomolar Concentrations by the Diffraction Pattern Imaging with Plasmonic Metasurfaces and Convex Holographic Gratings.

Compact and cost-effective optical devices for highly sensitive detection of trace molecules are significant in many applications, including healthcare, pollutant monitoring and explosive detection. Nanophotonic metasurface-based sensors have been intensively attracting attentions for molecular detection. However, conventional methods often involve spectroscopic characterizations that require bulky, expensive and sophisticated spectrometers. Here, a novel ultrasensitive sensor of plasmonic metasurfaces is designed and fabricated for the detection of trace molecules. The sensor features a convex holographic grating, of which the first-order diffraction pattern of a disposable metasurface is recorded by a monochrome camera.The diffraction pattern changes with the molecules attached to the metasurface, realizing label-free and spectrometer-free molecular detection by imaging and analyzing of the diffraction pattern. By integrating the sensor with a microfluidic setup, the quantitative characterization of rabbit anti-human Immunoglobulin G (IgG) and human IgG biomolecular interactions is demonstrated with an excellent limit of detection (LOD) of 0.6 pm. Moreover, both the metasurface and holographic grating are obtained through vacuum-free solution-processed fabrications, minimizing the manufacturing cost of the sensor. A prototype of the imaging-based sensor, consisting of a white light-emitting diode (LED) and a consumer-level imaging sensor is achieved to demonstrate the potential for on-site detection.

A high flexibility all-solid contact sulfide selective electrode using a graphene transducer.

In this paper, a novel high flexibility all-solid contact ion selective electrode (ASC-ISE) based on reduced graphene sheets (RGSs) as the ion-to-electron transducer was developed for rapid detection of sulfide. A graphene layer was firstly electrodeposited on a flexible silver wire by direct reduction of graphene oxide, and nanostructured Ag2S was then prepared as the selective membrane by electrodeposition. Scanning electrochemical microscopy was performed for the characterization of the morphological properties of the RGSs and Ag2S membranes. The evaluation of the analytical performances, such as the linear range, selectivity, stability, and practical application, of the proposed ASC-ISEs for the rapid detection of sulfide was performed. The results showed that, the ASC-ISEs exhibited a linear relationship between the obtained potential signal and sulfide concentration in the range of 0.50 µM to 1.0 mM, with a detection limit of 0.18 µM. Moreover, the ASC-ISEs showed good selectivity towards sulfide over other common interfering ions, and maintained a stable electrochemical response over 7 days. These results demonstrated that graphene was a promising material as the ion-to-electron transducer layer in the development of ASC-ISEs for sulfide detection, and the results of practical applications in tap water and seawater samples showed that the ASC-ISEs held significant promise in a broad range of applications.