Magnetically controlled graphene field-effect transistor biosensor for highly sensitive detection of cardiac troponin I.

Herein, we have constructed a magnetic graphene field-effect transistor biosensor (MGFETs) for highly sensitive detection of cardiac troponin I (CTNI). Graphene films transferred to ITO conductive glass as conductive channels. CTNI aptamer was immobilized onto the graphene film via 1-pyrene-butanoic acid succinimidyl ester (PBASE) to capture CTNI. Magnetic nanobeads (MBs) modified with CTNI antibody were added to the reaction chamber to form an aptamer/CTNI/antibody/magnetic nanobeads sandwich-type complex. We found that the magnetic force exerted on the complex leads to an impedance change of the graphene film. The reason for this result is that the magnetic field exerts an influence on the MBs, causing CTNI aptamer strand to bend, resulting in a change in the distance between the double conductive layers of the graphene film surface and the test solution. With periodic sampling integration, different concentrations of CTNI can be detected with high sensitivity. Due to the stringent recognition capability and high affinity between the CTNI aptamer and CTNI, MGFETs have the potential to detect various types of proteins. Furthermore, MGFETs also have the potential to be utilized for the detection of DNA or specific cells in the future.

Overcoming Debye length limitations: Three-dimensional wrinkled graphene field-effect transistor for ultra-sensitive adenosine triphosphate detection.

Adenosine triphosphate (ATP) is closely related to the pathogenesis of certain diseases, so the detection of trace ATP is of great significance to disease diagnosis and drug development. Graphene field-effect transistors (GFETs) have been proven to be a promising platform for the rapid and accurate detection of small molecules, while the Debye shielding limits the sensitive detection in real samples. Here, a three-dimensional wrinkled graphene field-effect transistor (3D WG-FET) biosensor for ultra-sensitive detection of ATP is demonstrated. The lowest detection limit of 3D WG-FET for analyzing ATP is down to 3.01 aM, which is much lower than the reported results. In addition, the 3D WG-FET biosensor shows a good linear electrical response to ATP concentrations in a broad range of detection from 10 aM to 10 pM. Meanwhile, we achieved ultra-sensitive (LOD: 10 aM) and quantitative (range from 10 aM to 100 fM) measurements of ATP in human serum. The 3D WG-FET also exhibits high specificity. This work may provide a novel approach to improve the sensitivity for the detection of ATP in complex biological matrix, showing a broad application value for early clinical diagnosis and food health monitoring. Electronic supplementary materials: The online version contains supplementary material available at 10.1007/s11467-023-1281-7 and https://journal.hep.com.cn/fop/EN/10.1007/s11467-023-1281-7.

LSP-SPP Coupling Structure Based on Three-Dimensional Patterned Sapphire Substrate for Surface Enhanced Raman Scattering Sensing.

Although the fabrication of controllable three-dimensional (3D) microstructures on substrates has been proposed as an effective solution for SERS, there remains a gap in the detection and manufacturability of 3D substrates with high performance. In this study, photolithography is adopted to obtain a pyramid-like array on a patterned sapphire substrate (PSS), with Al2O3 as the dielectric layer. In addition, silver nanoparticles (AgNPs) are used to decorate Au films to obtain mass-producible 3D SRES substrates. In the case of low fluorescence, the substrate realizes the coupling of localized surface plasmon polaritons (LSPs) and surface plasmon polaritons (SPPs), which is consistent with the simulation results obtained using the finite element method. The performance of the SERS substrate is evaluated using rhodamine 6G (R6G) and toluidine blue (TB) as probe molecules with detection limits of 10-11 M and 10-9 M, respectively. The substrate exhibits high hydrophobicity and excellent light-capturing capability. Moreover, it shows self-cleaning ability and long-term stability in practical applications. Allowing for the consistency of the composite substrate in the preparation process and the high reproducibility of the test results, it is considered to be promising for mass production.

Composite substrate of graphene/Ag nanoparticles coupled with a multilayer film for surface-enhanced Raman scattering biosensing.

In this paper, we designed a surface-enhanced Raman scattering (SERS) substrate for graphene/Ag nanoparticles (Ag NPs) bonded multilayer film (MLF) using the hybrid nanostructures composed of graphene and plasmonic metal components with significant plasmonic electrical effects and unique optical characteristics. This paper achieved the advantages of efficient utilization of electromagnetic field and reduction of fluorescence background based on the electromagnetic enhancement activity of Ag NPs and unique physical/chemical properties of graphene with zero gap structures. Au/Al2O3 was stacked periodically to construct MLF. As indicated by the electric field intensity at the Au/Al2O3 interface of the respective layer, bulk plasmon polariton (BPP) in the MLF was excited and coupled with localized surface plasmon (LSP) in the Ag NPs, which enhanced the electromagnetic field on the top-layer of SERS substrate. To measure the performance of the SERS substrate, rhodamine 6G (R6G) and malachite green (MG) were used as the probe molecules, with the detection limits of 10-11 M and 10-8 M, respectively. The SERS substrate had high sensitivity and uniformity, which indicated that it has a broad application prospect in the field of molecular detection.

An optic-fiber graphene field effect transistor biosensor for the detection of single-stranded DNA.

Herein, a graphene field effect transistor (GFET) was constructed on an optic fiber end face to develop an integrated optical/electrical double read-out biosensor, which was used to detect target single-stranded DNA (tDNA). Two isolated Au electrodes were, respectively, prepared as the drain and source at the ends of an optic fiber and coated with a graphene film to construct a field effect transistor (FET). Probe aptamers modified with fluorophore 6'-carboxy-fluorescein (6'-FAM) were immobilized on the graphene for specific capture of tDNA. Graphene oxide (GO) was introduced to quench 6'-FAM and construct a fluorescence biosensor. Thus, a dual GFET and fluorescence biosensor was integrated on the end-face of an optic fiber. Following synchronous detection by fluorescence and FET methods, results showed satisfactory sensitivity for DNA detection. Compared with conventional biosensors using a single sensing technology, these dual sensing integrated biosensors significantly improved the reliability and accuracy of DNA detection. Furthermore, this proposed technique provides both a new biosensor for single-stranded DNA detection and a strategy for designing multi-sensing integrated biosensors.

LSPR optical fiber biosensor based on a 3D composite structure of gold nanoparticles and multilayer graphene films.

In this paper, a localized surface-plasmon resonance (LSPR) biosensor, which uses a U-shaped multi-mode fiber (U-MMF), is introduced and investigated. It is modified with a complex of three-dimensional (3D) gold nanoparticles and multilayer graphene as spacer: n*(Au/G)@U-MMF, where n denotes the layer number of gold nanoparticles. The gold nanoparticles were synthesized by reducing chloroauric acid. Graphene films were formed using a liquid/chemical method. The number of gold-nanoparticle layers was found to be critical for the performance of the sensor. Moreover, using the finite-difference time domain, 3D nanostructures, with a wide range of gold-nanoparticle layers, were explored. The sensor showed the sensitivity of 1251.44 nm/RIU, as well as high stability and repeatability; for the measurement-process of time- and concentration-dependent DNA hybridization kinetics with detection concentrations, ranging from 0.1nM to 100 nM, the sensor displayed excellent performance, which points towards a vast potential in the field of medical diagnostics.

Preparation of Graphene/ITO Nanorod Metamaterial/U-Bent-Annealing Fiber Sensor and DNA Biomolecule Detection.

In this paper, a graphene/ITO nanorod metamaterial/U-bent-annealing (Gr/ITO-NM/U-bent-A)-based U-bent optical fiber local surface plasmon resonance (LSPR) sensor is presented and demonstrated for DNA detection. The proposed sensor, compared with other conventional sensors, exhibits higher sensitivity, lower cost, as well as better biological affinity and oxidize resistance. Besides, it has a structure of an original Indium Tin Oxides (ITO) nanocolumn array coated with graphene, allowing the sensor to exert significant bulk plasmon resonance effect. Moreover, for its discontinuous structure, a larger specific surface area is created to accommodate more biomolecules, thus maximizing the biological properties. The fabricated sensors exhibit great performance (690.7 nm/RIU) in alcohol solution testing. Furthermore, it also exhibits an excellent linear response (R2 = 0.998) to the target DNA with respective concentrations from 0.1 to 100 nM suggesting the promising medical applications of such sensors.

Magnetic Graphene Field-Effect Transistor Biosensor for Single-Strand DNA Detection.

Herein, a magnetic graphene field-effect transistor biosensor was prepared through the transfer of a chemical vapor deposition graphene film onto a glass substrate to produce a sensing film and conductive channel. By fixing 1-pyrenebutanoic acid succinimidyl ester onto graphene film as an anchor, a probe aptamer was immobilized on the graphene film in order to capture magnetically labeled complementary single-stranded DNA. Our experiments showed that, within a periodic magnetic field, the biosensor impedance exhibited a periodic oscillation, the amplitude of which was correlated to the complementary DNA concentration. Based on this principle, the magnetic graphene field-effect transistor was utilized to detect single-stranded DNA with detection limition of 1 pM. The results were rationalized using a model wherein the magnetic force causes the DNA strand to bend, thereby resulting in magnetic nanobeads/DNA modulation of the double conductive layer of graphene transistors. Furthermore, since a periodic magnetic field could be introduced to produce a periodic impedance changes of MGFETs, sampling integration could be used to improve the signal-to-noise ratio efficiently by increasing the number of periods of the external magnetic field. Therefore, a novel biosensor for DNA detection with high sensitivity has been presented in this work. Based on the detection principle, this system may also be a potential tool for detecting other bio-molecules, cells, etc.

Spin Polarization Properties of Pentagonal PdSe2 Induced by 3D Transition-Metal Doping: First-Principles Calculations.

The electronic structure and spin polarization properties of pentagonal structure PdSe2 doped with transition metal atoms are studied through first- principles calculations. The theoretical investigations show that the band gap of the PdSe2 monolayer decreases after introducing Cr, Mn, Fe and Co dopants. The projected densities of states show that p-d orbital couplings between the transition metal atoms and PdSe2 generate new spin nondegenerate states near the Fermi level which make the system spin polarized. The calculated magnetic moments, spin density distributions and charge transfer of the systems suggest that the spin polarization in Cr-doped PdSe2 will be the biggest. Our work shows that the properties of PdSe2 can be modified by doping transition metal atoms, which provides opportunity for the applications of PdSe2 in electronics and spintronics.

Optical Properties of Graphene/MoS2 Heterostructure: First Principles Calculations.

The electronic structure and the optical properties of Graphene/MoS2 heterostructure (GM) are studied based on density functional theory. Compared with single-layer graphene, the bandgap will be opened; however, the bandgap will be reduced significantly when compared with single-layer MoS2. Redshifts of the absorption coefficient, refractive index, and the reflectance appear in the GM system; however, blueshift is found for the energy loss spectrum. Electronic structure and optical properties of single-layer graphene and MoS2 are changed after they are combined to form the heterostructure, which broadens the extensive developments of two-dimensional materials.

A smartphone-based double-channel fluorescence setup for immunoassay of a carcinoembryonic antigen using CuS nanoparticles for signal amplification.

Sensitive detection of cancer biomarkers is valuable for clinical diagnosis and treatment assessment of cancers. Herein, we report a simple smartphone-based double-channel fluorescence setup for immunoassay. Not including the smartphone, the total cost of the detection device itself is about 80 $, including a laser pointer, a twinning measurement cell, a collective lens, and an outside box. The fluorescence images of the sample and reference areas were captured by the camera in the smartphone and the brightness ratio was calculated using a user-edited smartphone app. By using 2,3-diaminophenazine (DAP) as the model luminophore, the influence of exposure time and photosensitivity on the sensitivity was tested. The brightness ratio offers high stability of the fluorescence signal, which is helpful to improve the sensitivity. The applicability of this device was demonstrated by a catalytic fluorimetric method for Cu2+ determination, which is based on the oxidation of o-phenylenediamine (non-fluorescent) to DAP (strong fluorescent) by dissolved oxygen using Cu2+ as the catalyst. Accordingly, by using a CuS nanoparticle-conjugated second antibody as the signal tag, the immunoassay for a carcinoembryonic antigen was performed with the detection limit of 0.05 pg mL-1. This smartphone-based double-channel fluorescence device offers the advantages of high sensitivity, inexpensive and miniaturization.

Real-time reliable determination of binding kinetics of DNA hybridization using a multi-channel graphene biosensor.

Reliable determination of binding kinetics and affinity of DNA hybridization and single-base mismatches plays an essential role in systems biology, personalized and precision medicine. The standard tools are optical-based sensors that are difficult to operate in low cost and to miniaturize for high-throughput measurement. Biosensors based on nanowire field-effect transistors have been developed, but reliable and cost-effective fabrication remains a challenge. Here, we demonstrate that a graphene single-crystal domain patterned into multiple channels can measure time- and concentration-dependent DNA hybridization kinetics and affinity reliably and sensitively, with a detection limit of 10 pM for DNA. It can distinguish single-base mutations quantitatively in real time. An analytical model is developed to estimate probe density, efficiency of hybridization and the maximum sensor response. The results suggest a promising future for cost-effective, high-throughput screening of drug candidates, genetic variations and disease biomarkers by using an integrated, miniaturized, all-electrical multiplexed, graphene-based DNA array.

Theoretical Identification of Three C66 Fullerene Isomers and Related Chlorinated Derivatives by X-ray Photoelectron Spectroscopy and Near-edge X-ray Absorption Fine Structure Spectroscopy.

C 1s X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) spectra for three C66 fullerene isomers and related chlorinated species have been calculated by density functional theory (DFT) method. The XPS spectra show isomer dependence for the three pristine C66 isomers but not for the chlorinated species. The NEXAFS spectra exhibit strong dependence on the structures of all the investigated molecules and thus can be well employed to identify the three C66 fullerene isomers and related chlorinated species. Both XPS and NEXAFS spectra of the chlorinated species present significant variations compared with the pristine fullerenes. The spectral components for carbon atoms of different local environments have been explored as well. The spectra for the carbon atoms connecting to chlorine atoms exhibit a significant blue shift compared to the others.

Direct growth of graphene on quartz substrates for label-free detection of adenosine triphosphate.

We demonstrate that continuous, uniform graphene films can be directly synthesized on quartz substrates using a two-temperature-zone chemical vapor deposition system and that their layers can be controlled by adjusting the precursor partial pressure. Raman spectroscopy and transmission electron microscopy confirm the formation of monolayer graphene with a grain size of ∼100 nm. Hall measurements show a room-temperature carrier mobility above 1500 cm2 V(-1) s(-1). The optical transmittance and conductance of the graphene films are comparable to those of transferred metal-catalyzed graphene. The method avoids the complicated and skilled post-growth transfer process and allows the graphene to be directly incorporated into a fully functional biosensor for label-free detection of adenosine triphosphate (ATP). This device shows a fast response time of a few milliseconds and achieves a high sensitivity to ATP molecules over a very wide range from 0.002 to 5 mM.

[Testosterone level not significantly correlates to endothelial progenitor cells in Klinefelter's syndrome patients].

OBJECTIVE: To explore the correlation of the testosterone level with circulated endothelial progenitor cells in patients with Klinefelter's syndrome (KS) and its clinical significance. METHODS: This study included 36 patients affected by non-mosaic 47, XXY KS, each with one or more cardiovascular risk factors. Serum hormone levels and the content of circulated endothelial progenitor cells were determined by radioimmunology and cell culture methods, respectively, and the measurement was repeated after 6 months of testosterone replacement therapy. RESULTS: After testosterone replacement therapy, the testosterone level was increased from (8 +/- 3) to (24 +/- 10) nmol/L, while the content of endothelial progenitor cells ([41 +/- 48] cells/ml) showed no significant rise. CONCLUSION: There is no obvious correlation between the testosterone level and the content of endothelial progenitor cells in KS patients.

Disposable bioluminescence-based biosensor for detection of bacterial count in food.

A biosensor for rapid detection of bacterial count based on adenosine 5'-triphosphate (ATP) bioluminescence has been developed. The biosensor is composed of a key sensitive element and a photomultiplier tube used as a detector element. The disposable sensitive element consists of a sampler, a cartridge where intracellular ATP is chemically extracted from bacteria, and a microtube where the extracted ATP reacts with the luciferin-luciferase reagent to produce bioluminescence. The bioluminescence signal is transformed into relevant electrical signal by the detector and further measured with a homemade luminometer. Parameters affecting the amount of the extracted ATP, including the types of ATP extractants, the concentrations of ATP extractant, and the relevant neutralizing reagent, were optimized. Under the optimal experimental conditions, the biosensor showed a linear response to standard bacteria in a concentration range from 10(3) to 10(8) colony-forming units (CFU) per milliliter with a correlation coefficient of 0.925 (n=22) within 5min. Moreover, the bacterial count of real food samples obtained by the biosensor correlated well with those by the conventional plate count method. The proposed biosensor, with characteristics of low cost, easy operation, and fast response, provides potential application to rapid evaluation of bacterial contamination in the food industry, environment monitoring, and other fields.