ABSTRACT
The accurate diagnosis of diabetic nephropathy relies on achieving ultrasensitive biosensing for biomarker detection. However, existing biosensors face challenges such as poor sensitivity, complexity, time-consuming procedures, and high assay costs. To address these limitations, we report a WS2-based plasmonic biosensor for the ultrasensitive detection of biomarker candidates in clinical human urine samples associated with diabetic nephropathy. Leveraging plasmonic-based electrochemical impedance microscopy (P-EIM) imaging, we observed a remarkable charge sensitivity in monolayer WS2 single crystals. Our biosensor exhibits an exceptionally low detection limit (0.201 ag/mL) and remarkable selectivity in detecting CC chemokine ligand 2 (CCL2) protein biomarkers, outperforming conventional techniques such as ELISA. This work represents a breakthrough in traditional protein sensors, providing a direction and materials foundation for developing ultrasensitive sensors tailored to clinical applications for biomarker sensing.
Subject(s)
Biomarkers , Biosensing Techniques , Chemokine CCL2 , Diabetic Nephropathies , Humans , Diabetic Nephropathies/urine , Diabetic Nephropathies/diagnosis , Biosensing Techniques/methods , Chemokine CCL2/urine , Biomarkers/urine , Limit of Detection , Electrochemical Techniques/methodsABSTRACT
Chiral alkyl chains are ubiquitously observed in organic semiconductor materials and can regulate solution processability and active layer morphology, but the effect of stereoisomers on photovoltaic performance has rarely been investigated. For the racemic Y-type acceptors widely used in organic solar cells, it remains unknown if the individual chiral molecules separate into the conglomerate phase or if racemic phase prevails. Here, the photovoltaic performance of enantiomerically pure Y6 derivatives, (S,S)/(R,R)-BTP-4F, and their chiral mixtures are compared. It is found that (S,S) and (R,R)-BTP-4F molecule in the racemic mixtures tends to interact with its enantiomer. The racemic mixtures enable efficient light harvesting, fast hole transfer, and long polaron lifetime, which is conducive to charge generation and suppresses the recombination losses. Moreover, abundant charge diffusion pathways provided by the racemate contribute to efficient charge transport. As a result, the racemate system maximizes the power output and minimizes losses, leading to a higher efficiency of 18.16% and a reduced energy loss of 0.549 eV, as compared to the enantiomerically pure molecules. This study demonstrates that the chirality of non-fullerene acceptors should receive more attention and be designed rationally to enhance the efficiency of organic solar cells.
ABSTRACT
Ultrasensitive detection of biomarkers, particularly proteins, and microRNA, is critical for disease early diagnosis. Although surface plasmon resonance biosensors offer label-free, real-time detection, it is challenging to detect biomolecules at low concentrations that only induce a minor mass or refractive index change on the analyte molecules. Here an ultrasensitive plasmonic biosensor strategy is reported by utilizing the ferroelectric properties of Bi2O2Te as a sensitive-layer material. The polarization alteration of ferroelectric Bi2O2Te produces a significant plasmonic biosensing response, enabling the detection of charged biomolecules even at ultralow concentrations. An extraordinary ultralow detection limit of 1 fm is achieved for protein molecules and an unprecedented 0.1 fm for miRNA molecules, demonstrating exceptional specificity. The finding opens a promising avenue for the integration of 2D ferroelectric materials into plasmonic biosensors, with potential applications spanning a wide range.
Subject(s)
Biosensing Techniques , Surface Plasmon Resonance , Biosensing Techniques/methods , Surface Plasmon Resonance/methods , Bismuth/chemistry , MicroRNAs/analysisABSTRACT
Non-fullerene acceptor molecules developed for organic solar cells feature a very intense absorption band in the near-infrared. In the solid phase, the strong interaction between light and the transition dipole moment for molecular excitation should induce formation of polaritons. The reflection spectra for polycrystalline films of a non-fullerene acceptor with a thienothienopyrrolo-thienothienoindole core of the so-called Y6 type indeed show a signature of polaritons. A local minimum in the middle of the reflection band is associated with the allowed molecular transition. The minimum in reflection allows efficient entry of light into the solid, resulting in a local maximum in external quantum efficiency of a photovoltaic cell made of the pure acceptor.
ABSTRACT
Plasmonic biosensing is a label-free detection method that is commonly used to measure various biomolecular interactions. However, one of the main challenges in this approach is the ability to detect biomolecules at low concentrations with sufficient sensitivity and detection limits. Here, 2D ferroelectric materials are employed to address the issues with sensitivity in biosensor design. A plasmonic sensor based on Bi2 O2 Se nanosheets, a ferroelectric 2D material, is presented for the ultrasensitive detection of the protein molecule. Through imaging the surface charge density of Bi2 O2 Se, a detection limit of 1 fM is achieved for bovine serum albumin (BSA). These findings underscore the potential of ferroelectric 2D materials as critical building blocks for future biosensor and biomaterial architectures.
ABSTRACT
2D materials with low symmetry are explored in recent years because of their anisotropic advantage in polarization-sensitive photodetection. Herein the controllably grown hexagonal magnetic semiconducting α-MnTe nanoribbons are reported with a highly anisotropic (100) surface and their high sensitivity to polarization in a broadband photodetection, whereas the hexagonal structure is highly symmetric. The outstanding photoresponse of α-MnTe nanoribbons occurs in a broadband range from ultraviolet (UV, 360 nm) to near infrared (NIR, 914 nm) with short response times of 46 ms (rise) and 37 ms (fall), excellent environmental stability, and repeatability. Furthermore, due to highly anisotropic (100) surface, the α-MnTe nanoribbons as photodetector exhibit attractive sensitivity to polarization and high dichroic ratios of up to 2.8 under light illumination of UV-to-NIR wavelengths. These results demonstrate that 2D magnetic semiconducting α-MnTe nanoribbons provide a promising platform to design the next-generation polarization-sensitive photodetectors in a broadband range.
ABSTRACT
Organic photodetectors that can sensitively convert near-infrared (NIR) circularly polarized light (CPL) into modulable electrical signals have promising applications in spectroscopy, imaging, and communications. However, the preparation of chiral NIR organic photodetectors with simultaneously high dissymmetry factor, responsivity, detectivity, and response speed is challenging. Here, direct CPL detectors based on the bulk heterojunctions (BHJs) of chiral BTP-4Cl non-fullerene acceptor with dilute achiral PM6 donor are constructed, which successfully address these issues. The chiral acceptor-enriched BHJs with a donor/acceptor ratio of 1/10 achieve an optimal trade-off between chiroptical properties and optoelectronic performance. The supramolecular chirality from the acceptor aggregates provides the BHJs with a true absorption dissymmetry factor (gabs ) of ±0.02 at 830 nm, the highest value among NIR-sensitive detectors, which endows the photodetector with a photocurrent dissymmetry factor (gsc ) of ±0.03. Impressively, the photodetector demonstrates an external quantum efficiency as high as 60%, a responsivity of 0.4 A W-1 , a detectivity of 3 × 1011 Jones (based on noise current), and a fast response speed on the microsecond scale with the -3 dB bandwidth over 7000 Hz in the NIR region. This study exhibits a promising strategy for building high-performing direct NIR CPL detectors by introducing supramolecular chirality into BHJs.
ABSTRACT
Increased matrix metalloproteinase 9 (MMP9) expression is involved in delayed wound healing in diabetic foot ulcers. We created skin wounds in normal SD rats and STZ-induced diabetic SD rats, then we found protein levels of activator protein-1 (AP1), a crucial transcription factor to increase MMP9 transcription, as well as MMP9 was up-regulated in epithelium of diabetic skin tissues. Then, we evaluated the mRNA and protein stability of AP1 subunits C-FOS/C-Jun in HaCaT cells after high glucose treatment. Results showed that high glucose could increase protein stability of C-FOS and C-Jun. Additionally, high glucose also activated extracellular signaling-related kinase 1/2 (ERK1/2). ERK1/2 inhibitor could rescue phosphorylation of C-FOS and C-Jun, increased protein stability of C-Jun, and increased MMP9 expressions. Thus, our study demonstrated that high glucose could activate ERK1/2 to stabilize AP1 and increase MMP9 expression in diabetic skin and HaCaT cells.
Subject(s)
Diabetic Foot/drug therapy , Glucose/pharmacology , Matrix Metalloproteinase 9/metabolism , Transcription Factor AP-1/metabolism , Animals , Diabetes Mellitus/drug therapy , Diabetic Foot/metabolism , Humans , JNK Mitogen-Activated Protein Kinases/drug effects , JNK Mitogen-Activated Protein Kinases/metabolism , MAP Kinase Signaling System/drug effects , Mitogen-Activated Protein Kinases/drug effects , Mitogen-Activated Protein Kinases/metabolism , Rats, Sprague-Dawley , Signal Transduction/drug effects , Transcription Factor AP-1/drug effects , Up-Regulation/drug effectsABSTRACT
Seeded lithium (Li) nucleation has been considered as a promising strategy to achieve uniform Li deposition. However, problems of agglomeration and pulverization quickly invalidate the nucleation seeds, resulting in Li dendrite growth during repeated charge/discharge processes. Herein, liquid gallium-indium (GaIn) nanoparticles with structural self-healing properties are utilized to guide uniform metallic Li nucleation and deposition. Ultrafine GaIn nanoparticles (â¼25 nm) uniformly decorated on the surface of carbon layers effectively homogenize the lithium-ion flux. After fully Li stripping, lithiophilic GaIn nanoparticles return to the liquid binary eutectic phase, thereby healing the deformed structure and enabling them to continuously guide dendrite-free Li deposition. Li metal anodes with such nucleation seeds exhibit nearly zero nucleation overpotential even after hundreds of cycles and a high average Coulombic efficiency of 99.03% for more than 400 cycles. The design of self-healing nucleation seeds provides important insights for obtaining high-performance lithium metal anodes.
ABSTRACT
Vascular calcification is closely linked to patients in diabetes mellitus and chronic kidney disease. Advanced glycation end-products (AGEs) are associated with osteogenic differentiation of vascular smooth muscle cell (VSMC), vascular calcification, and autophagy that takes part in the process. However, the underlying mechanism of the effects of AGEs on the phenotypic transition and autophagy of VSMCs is not clearly understood. In this study, we cultured the rat VSMC line (A7R5) and thoracic aorta organ with bovine serum albumin (BSA) or AGEs (AGEs-BSA) and detected proteins expression by Western blotting or immunofluorescence. Autophagosome was observed by transmission electron microscopy (TEM). The mineralization and calcific nodules were identified by Alizarin Red S and Von Kossa staining. AGEs significantly downregulated p-AMPKα expression and upregulated p-mTOR expression and then increased the expression of osteoblastic differentiation, while suppressing autophagy in a time-dependent pattern. Pretreatment with autophagy activator rapamycin and AMPK activator AICAR both upregulated the autophagy level and downregulated the effects of AGEs on osteoblastic differentiation of VSMCs. Moreover, the result from rat thoracic aorta culture also confirmed that AGEs promote vascular calcification in a time-dependent manner. Thus, our study showed that AGEs quicken vascular calcification and suppress autophagy associated with AMPK/mTOR signaling pathway.
Subject(s)
AMP-Activated Protein Kinases/metabolism , Autophagy , Glycation End Products, Advanced/metabolism , Osteogenesis , TOR Serine-Threonine Kinases/metabolism , Vascular Calcification/pathology , Animals , Cell Differentiation , Cells, Cultured , Male , Muscle, Smooth, Vascular/metabolism , Rats , Rats, Sprague-Dawley , Signal Transduction , Vascular Calcification/metabolismABSTRACT
Adenosine is a promising cytotoxic reagent for tumors, long noncoding RNA (lncRNA) maternally expressed gene 3 (MEG3) has been indicated to play critical roles in tumorigenesis, ILF3 has been recognized as a MEG3-binding protein, however, the roles of adenosine and MEG3 on hepatoma are still ambiguous. To clarify the effects of MEG3 on the adenosine-induced cytotoxicity in hepatoma, MEG3 and ILF3 lentivirus were transduced into human hepatoma HepG2 cells to stimulate overexpression of MEG3 (OE MEG3) and overexpression of ILF3 (OE ILF3), furthermore, ILF3 small interfering RNA (siRNA) was also applied to downregulate the expression of ILF3. In this study, autophagy was markedly inhibited by low concentration of adenosine, which present by not only inhibited transformation from LC3-I to LC3-II and autophagosomes formation, but also the elevation of mTOR and reduction of beclin-1 proteins. Furthermore, low concentration of adenosine also exerted marked cytotoxicity representing induced cell apoptosis together with reductions of cell viability and migration, which were also markedly enhanced by OE MEG3. Novelly and excitingly, adenosine markedly stimulated MEG3 expression, OE MEG3 markedly decreased the ILF3 expression in HepG2 cells, and the adenosine-induced autophagy inhibition, together with the ratio of p-PI3K/PI3K, p-AKT/AKT, and p-mTOR/mTOR were also boosted by OE MEG3. More interestingly, OE ILF3 increased autophagy, whereas downregulated ILF3, especially in the case of adenosine, led to marked autophagy inhibition by decreasing beclin-1. The present study demonstrates autophagy inhibition is involved in the adenosine-induced cytotoxicity in HepG2 cells, the cytotoxicity can be synergized by OE MEG3 via downregulated ILF3 to activate PI3K/Akt/mTOR and inactivate the beclin-1 signaling pathway. In conclusion, MEG3 and inhibition of autophagy might be potential targets for augmenting adenosine-induced cytotoxicity in hepatoma.
Subject(s)
Adenosine/pharmacology , Autophagy/drug effects , Beclin-1/metabolism , Nuclear Factor 90 Proteins/genetics , Phosphotransferases/metabolism , RNA, Long Noncoding/genetics , Signal Transduction/drug effects , Apoptosis/drug effects , Apoptosis/genetics , Autophagy/genetics , Carcinoma, Hepatocellular/genetics , Carcinoma, Hepatocellular/metabolism , Carcinoma, Hepatocellular/pathology , Cell Survival/drug effects , Cell Survival/genetics , Down-Regulation/drug effects , Gene Expression Regulation, Neoplastic/drug effects , Gene Expression Regulation, Neoplastic/genetics , Hep G2 Cells , Humans , Liver Neoplasms/genetics , Liver Neoplasms/metabolism , Liver Neoplasms/pathology , Nuclear Factor 90 Proteins/metabolism , Phosphatidylinositol 3-Kinases/metabolism , Proto-Oncogene Proteins c-akt/metabolism , Signal Transduction/genetics , TOR Serine-Threonine Kinases/metabolismABSTRACT
Domain boundaries have been intensively investigated in bulk ferroelectric materials and two-dimensional materials. Many methods such as electrical, mechanical and optical approaches have been utilized to probe and manipulate domain boundaries. So far most research focuses on the initial and final states of domain boundaries before and after manipulation, while the microscopic understanding of the evolution of domain boundaries remains elusive. In this paper, we report controllable manipulation of the domain boundaries in two-dimensional ferroelectric In2Se3 with atomic precision using scanning tunneling microscopy. We show that the movements of the domain boundaries can be driven by the electric field from a scanning tunneling microscope tip and proceed by the collective shifting of atoms at the domain boundaries. Our density functional theory calculations reveal the energy path and evolution of the domain boundary movement. The results provide deep insight into domain boundaries in two-dimensional ferroelectric materials and will inspire inventive applications of these materials.
ABSTRACT
Imaging the surface charge of biomolecules such as proteins and DNA, is crucial for comprehending their structure and function. Unfortunately, current methods for label-free, sensitive, and rapid imaging of the surface charge of single DNA molecules are limited. Here, we propose a plasmonic microscopy strategy that utilizes charge-sensitive single-crystal monolayer WS2 materials to image the local charge density of a single λ-DNA molecule. Our study reveals that WS2 is a highly sensitive charge-sensitive material that can accurately measure the local charge density of λ-DNA with high spatial resolution and sensitivity. The consistency of the surface charge density values obtained from the single-crystal monolayer WS2 materials with theoretical simulations demonstrates the reliability of our approach. Our findings suggest that this class of materials has significant implications for the development of label-free, scanning-free, and rapid optical detection and charge imaging of biomolecules.
Subject(s)
DNA , DNA/chemistry , Tungsten Compounds/chemistry , Microscopy/methodsABSTRACT
2D magnetic materials hold substantial promise in information storage and neuromorphic device applications. However, achieving a 2D material with high Curie temperature (TC), environmental stability, and multi-level magnetic states remains a challenge. This is particularly relevant for spintronic devices, which require multi-level resistance states to enhance memory density and fulfil low power consumption and multi-functionality. Here, the synthesis of 2D non-layered triangular and hexagonal magnetite (Fe3O4) nanosheets are proposed with high TC and environmental stability, and demonstrate that the ultrathin triangular nanosheets show broad antiphase boundaries (bAPBs) and sharp antiphase boundaries (sAPBs), which induce multiple spin precession modes and multi-level resistance. Conversely, the hexagonal nanosheets display slip bands with sAPBs associated with pinning effects, resulting in magnetic-field-driven spin texture reversal reminiscent of "0" and "1" switching signals. In support of the micromagnetic simulation, direct explanation is offer to the variation in multi-level resistance under a microwave field, which is ascribed to the multi-spin texture magnetization structure and the randomly distributed APBs within the material. These novel 2D magnetite nanosheets with unique spin textures and spin dynamics provide an exciting platform for constructing real multi-level storage devices catering to emerging information storage and neuromorphic computing requirements.
ABSTRACT
Two-dimensional transition metal dichalcogenide (TMDC) heterostructure is receiving considerable attention due to its novel electronic, optoelectronic, and spintronic devices with design-oriented and functional features. However, direct design and synthesis of high-quality TMDC/MnTe heterostructures remain difficult, which severely impede further investigations of semiconductor/magnetic semiconductor devices. Herein, the synthesis of high-quality vertically stacked WS2/MnTe heterostructures is realized via a two-step chemical vapor deposition method. Raman, photoluminescence, and scanning transmission electron microscopy characterizations reveal the high-quality and atomically sharp interfaces of the WS2/MnTe heterostructure. WS2/MnTe-based van der Waals field effect transistors demonstrate high rectification behavior with rectification ratio up to 106, as well as a typical p-n electrical transport characteristic. Notably, the fabricated WS2/MnTe photodetector exhibits sensitive and broadband photoresponse ranging from UV to NIR with a maximum responsivity of 1.2 × 103 A/W, a high external quantum efficiency of 2.7 × 105%, and fast photoresponse time of â¼50 ms. Moreover, WS2/MnTe heterostructure photodetectors possess a broadband image sensing capability at room temperature, suggesting potential applications in next-generation high-performance and broadband image sensing photodetectors.
ABSTRACT
Detection of the circular polarization of light is possible using chiral semiconductors, yet the mechanisms remain poorly understood. Semi-transparent chiral photodiodes allow for a simple experiment to investigate the basis of their selectivity: changing the side from which the diode is illuminated. A reversal of circular selectivity is observed in photocurrent generation when changing the direction of illumination on organic, bulk-heterojunction cells. The change in selectivity can be explained by a space-charge limitation on the collection of photocarriers in combination with preferential absorption of one of the circular polarizations of near-infrared light by the chiral non-fullerene acceptor. The space-charge limitation is supported by detailed measurements of frequency and intensity dependence of dc and ac photocurrents.
ABSTRACT
OBJECTIVES: Mutation in human FAM134B gene has been implicated in hereditary sensory and autonomic neuropathy type IIB. We aimed to knock out Fam134b in mice and explored its phenotypes to determine whether the genetic impairments and behavioral changes can mirror manifestations noted in humans. METHODS: We used CRISPR/Cas9 technology to knockout the Fam134b gene in the C57BL/6 J mouse. After confirming the knockout was successful by Sanger sequencing and Western blot, sensory function was measured using the hot plate test and the 50% paw withdrawal threshold test. In addition, standard microscopy and transmission electron microscopy were performed to observe the structural changes of the dorsal root ganglion sensory neuron and the sciatic nerve. RESULTS: DNA sequencing and Western blot analysis confirmed the mutation in the Fam134b mutation gene and the loss of expression of its products. Fam134b knockout mice exhibited heat pain insensitivity and mechanical hyperalgesia. Interestingly, limb damage was found in some homozygotes. Demyelination in the sciatic nerve was common. Golgi bodies were turgid in dorsal root ganglion neuron. CONCLUSIONS: These findings indicate that peripheral neuropathy is common in Fam134b KO mice. We believe this novel animal model is likely to have significant future potential as a reliable model for the evaluation of peripheral neuropathy and its complications.
Subject(s)
Hyperalgesia , Neurons , Mice , Humans , Animals , Mice, Knockout , Mice, Inbred C57BL , Neurons/metabolism , Hyperalgesia/metabolism , MutationABSTRACT
Supramolecular chiral organization gives π-conjugated molecules access to fascinating specific interactions with circularly polarized light (CPL). Such a feature enables the fabrication of high-performance chiral organic electronic devices that detect or emit CPL directly. Herein, it is shown that chiral fused-ring electron-acceptor BTP-4F single-crystal-based phototransistors demonstrate distinguished CPL discrimination capability with current dissymmetry factor exceeding 1.4, one of the highest values among state-of-the-art direct CPL detectors. Theoretical calculations prove that the chirality at the supramolecular level in these enantiomeric single crystals originates from chiral exciton coupling of a unique quasi-2D supramolecular organization consisting of interlaced molecules with opposite helical conformation. Impressively, such supramolecular organization produces a higher dissymmetry factor along the preferred growth direction of the chiral single crystals in comparison to that of the short axis direction. Furthermore, the amplified, inverted, and also anisotropic current dissymmetry compared to optical dissymmetry is studied by finite element simulations. Therefore, a unique chiral supramolecular organization that is responsible for the excellent chiroptical response and anisotropic electronic properties is developed, which not only enables the construction of high-performance CPL detection devices but also allows a better understanding of the structure-property relationships in chiral organic optoelectronics.
ABSTRACT
Among novel two-dimensional materials, transition metal dichalcogenides (TMDs) with 3dmagnetic elements have been extensively researched owing to their unique magnetic, electric, and photoelectric properties. As an important member of TMDs, CoSe2is an interesting material with controversial magnetic properties, hitherto there are few reports related to the magnetism of CoSe2materials. Here, we report the synthesis of CoSe2nanoplates on Al2O3substrates by chemical vapor deposition (CVD). The CVD-grown CoSe2nanoplates exhibit three typical morphologies (regular hexagonal, hexagonal, and pentagonal shapes) and their lateral sizes and thickness of CoSe2nanoplates can reach up to hundreds of microns and several hundred nanometers, respectively. The electric-transport measurement shows a metallic feature of CoSe2nanoplates. Furthermore, the slanted hysteresis loop and nonzero remnant magnetization of the CoSe2nanoplates confirm the ferromagnetism in the temperature range of 5-400 K. This work provides a novel platform for designing CoSe2-based spintronic devices and studying related magnetic mechanisms.
ABSTRACT
Ultrasensitive and rapid detection of biomarkers is among the upmost priorities in promoting healthcare advancements. Improved sensitivity of photonic sensors based on two-dimensional (2D) materials have brought exciting prospects for achieving real-time and label-free biosensing at dilute target concentrations. Here, we report a high-sensitivity surface plasmon resonance (SPR) RNA sensor using metallic 2D GeP5 nanosheets as the sensing material. Theoretical evaluations revealed that the presence of GeP5 nanosheets can greatly enhance the plasmonic electric field of the Au film thereby boosting sensing sensitivity, and that optimal sensitivity (146° RIU-1) can be achieved with 3-nm-thick GeP5. By functionalizing GeP5 nanosheets with specific cDNA probes, detection of SARS-CoV-2 RNA sequences were achieved using the GeP5-based SPR sensor, with high sensitivity down to a detection limit of 10 aM and excellent selectivity. This work demonstrates the immense potential of GeP5-based SPR sensors for advanced biosensing applications and paves the way for utilizing GeP5 nanosheets in novel sensor devices.