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1.
Opt Express ; 32(8): 13851-13863, 2024 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-38859344

RESUMO

This paper introduces an innovative, compact, and high-gain metasurface antenna, covering both the 24 GHz millimeter wave (mmWave) radar band and the 5 G n257 and n258 bands. The proposed metasurface antenna consists of a wideband stacked patch antenna and a dual-layer metasurface to focus its radiation beams for multiple mmWave bands. The operating frequency can be slightly shifted by altering the distance between the feeder and the metasurface. The distribution of the metasurface unit cells is designed based on a simplified phase compensation formula. The dimension of the fabricated feeder is 6 mm × 6 mm, and the metasurface occupies a 65 mm × 65 mm radome area. Experimental results demonstrate a wide bandwidth from 23.5 GHz to 29.1 GHz for the feeder, and impressive maximum gains of 19.7 dBi and 19.5 dBi for the lower band and higher band of the metasurface antenna are achieved simultaneously. The frequency reconfiguration ability was characterized by a 750 MHz frequency shift with every 1 mm distance adjustment. The compact size and high gain performance of the proposed design underscore its potential for practical applications in millimeter wave joint communication and radar sensing systems.

2.
Anal Chem ; 96(4): 1427-1435, 2024 01 30.
Artigo em Inglês | MEDLINE | ID: mdl-38226591

RESUMO

Although porphyrins make up a promising class of electrochemiluminescence (ECL) luminophors, their aggregation-caused quenching (ACQ) characteristics lead to inferior ECL efficiency (ΦECL). Furthermore, current application of porphyrins is limited to cathodic emission. This work creatively exploited a cage-like porous complex (referred to as SWU-1) as the microreactor to recede the ACQ effect while modulating dual ECL emission of meso-tetra(4-carboxyphenyl)porphine (TCPP), which self-assembled with SWU-1 to form TCPP@SWU-1 nanocapsules (TCPP@SWU-1 NCs). As the microreactor, SWU-1 not only effectively constrained TCPP aggregation to improve electron-hole recombination efficiency but also improved stability of anion and cation radicals, thus significantly enhancing the dual emission of TCPP. Compared with TCPP aggregates, the resulting TCPP@SWU-1 NCs exhibited significantly enhanced anodic and cathodic emission, and their ΦECL was increased by 8.7-fold and 3.9-fold, respectively. Furthermore, black hole quencher-2 (BHQ2) can simultaneously quench anodic and cathodic signals. TCPP@SWU-1 NCs coupling BHQ2 conveniently achieved an ECL ratio detection of miRNA-126, and the limit of detection (S/N = 3) was 4.1 aM. This work pioneered the development of the cage-like porous complex SWU-1 as the microreactor to alleviate defects of the ACQ effect and mediate dual emission of TCPP. The coupling of dual-emitting TCPP@SWU-1 NCs and dual-function moderator BHQ2 created a novel single-luminophor-based ratio system for bioanalysis and provided a promising ECL analysis approach for miRNA-126.


Assuntos
Técnicas Biossensoriais , MicroRNAs , Porfirinas , Porosidade , Fotometria , Medições Luminescentes/métodos , Técnicas Eletroquímicas/métodos
3.
Rev Sci Instrum ; 94(4)2023 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38081251

RESUMO

A cold collision between atoms and molecules (<1 K) is one of the hot research fields in atomic and molecular physics. At low temperatures, the number of partial waves participating in the collision process decreases dramatically, and quantum phenomena start to emerge. The reaction is often dominated by quantum tunneling, and pronounced resonances can exist on collision cross sections. Here, we report on an apparatus designed for studying cold collisions between metastable noble gas atoms and alkali atoms. Our apparatus features a combined Magneto-Optical-Trap (MOT) and velocity map imaging (VMI) system. The center of a Rb MOT is overlapped with the VMI system. Cold Kr* atoms are launched toward the Rb atoms to induce Kr* + Rb reactions. The collision energy between the two species can be varied from 100 mK to 20 K. With this setup, we are planning to explore the quantum phenomena in Kr* + Rb cold collisions, including the shape resonance and stereodynamics in the reaction.

4.
Anal Chem ; 95(49): 18207-18214, 2023 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-38010370

RESUMO

Owing to excellent catalytic activity, single-atom catalysts (SACs) have recently attracted considerable research interest in the electrochemiluminescence (ECL) field. However, the applications of SACs are mostly limited to conventional luminol ECL system. Hence, it is necessary to explore the application of SACs in more ECL systems. In this work, nickel single-atom catalysts (Ni SACs) were successfully applied in the graphitic carbon nitride (g-C3N4)-H2O2 ECL system to significantly enhance its cathodic emission. Notably, g-C3N4 acted not only as an ECL luminophore but also as a support to anchor Ni SACs. Ni SACs can significantly activate H2O2 to produce abundant OH• radicals for enhancing the cathodic ECL emission of g-C3N4. Ni SACs-anchored g-C3N4 (Ni SACs@g-C3N4) had a 10-fold enhanced ECL intensity as compared to g-C3N4. Finally, the Ni SACs@g-C3N4-H2O2 ECL system was developed to detect hepatitis B virus (HBV) DNA by incorporating an entropy-driven DNA walking machine-assisted CRISPR-Cas12a amplification strategy. The constructed biosensor exhibited excellent detection performance for HBV DNA with a limit of detection as low as 17 aM. This work puts forward a new idea for enhancing the cathodic ECL of g-C3N4-H2O2 and expands the application of SACs in the ECL system.


Assuntos
Técnicas Biossensoriais , DNA Viral , Níquel , Técnicas Eletroquímicas , Peróxido de Hidrogênio , Medições Luminescentes , Limite de Detecção
5.
Biosens Bioelectron ; 237: 115539, 2023 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-37487285

RESUMO

Constructing mono-luminophor-based electrochemiluminescence (ECL) ratio system is a great challenge due to the limitations of the luminescent species with dual-signal-output, luminescence efficiency and coreactant. This work developed carboxyl-functionalized poly[9,9-bis(3'-(N,N-dimethylamino) propyl)-2,7-fluorene]-alt-2,7-(9,9 dioctylfluorene)] nanoparticles(PFN NPs) as dual-emitting luminophors, which can synchronously output strong cathodic and anodic ECL signals without any exogenous coreactants. The inherent molecular structure enabled efficient intramolecular electron transfer between tertiary amine groups and backbone of PFN to generate strong cathodic and anodic ECL emission. Particularly, H+ in aqueous solution played an irreplaceable role for cathodic ECL emission. The silver nanoparticles (AgNPs) were developed as signal regulator because of their excellent hydrogen evolution reaction (HER) activity, which significantly quenched the cathodic signal while kept the anodic signal unchanged. The dual-emitting PFN NPs cleverly integrated signal regulator AgNPs and bicyclic strand displacement amplification (SDA) to construct a coreactant-free mono-luminophor-based ratiometric ECL sensing for SARS-CoV-2 RdRp gene assay. The strong dual-emitting of PFN NPs and excellent quenching effect of AgNPs on cathodic emission endowed the biosensor with a high detection sensitivity, and the detection limit was as low as 39 aM for RdRp gene. The unique dual-emitting properties of PFN NPs open up a new path to construct coreactant-free mono-luminophor-based ECL ratio platform, and excellent HER activity of AgNPs offers some new thoughts for realizing ECL signal changes.


Assuntos
Técnicas Biossensoriais , COVID-19 , Nanopartículas Metálicas , Humanos , Polímeros/química , Nanopartículas Metálicas/química , SARS-CoV-2/genética , Medições Luminescentes , COVID-19/diagnóstico , Prata , RNA Polimerase Dependente de RNA , Técnicas Eletroquímicas
6.
Rev Sci Instrum ; 94(3): 033202, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-37012821

RESUMO

We describe a high intensity metastable Kr source based on a helical resonator RF discharge. By adding an external B-field to the discharge source, the metastable Kr flux is enhanced. The effect of geometric configuration and magnetic field strength has been studied and optimized experimentally. Compared to the helical resonator discharge source without an external B-field, the new source showed an enhancement factor of 4-5 in producing metastable Kr beams. This improvement has a direct impact on the radio-krypton dating applications as it can increase the atom count rate, resulting in a higher analytical precision.

7.
Cell Rep ; 42(5): 112417, 2023 05 30.
Artigo em Inglês | MEDLINE | ID: mdl-37074913

RESUMO

The P-type ATPase ATP7B exports cytosolic copper and plays an essential role in the regulation of cellular copper homeostasis. Mutants of ATP7B cause Wilson disease (WD), an autosomal recessive disorder of copper metabolism. Here, we present cryoelectron microscopy (cryo-EM) structures of human ATP7B in the E1 state in the apo, the putative copper-bound, and the putative cisplatin-bound forms. In ATP7B, the N-terminal sixth metal-binding domain (MBD6) binds at the cytosolic copper entry site of the transmembrane domain (TMD), facilitating the delivery of copper from the MBD6 to the TMD. The sulfur-containing residues in the TMD of ATP7B mark the copper transport pathway. By comparing structures of the E1 state human ATP7B and E2-Pi state frog ATP7B, we propose the ATP-driving copper transport model of ATP7B. These structures not only advance our understanding of the mechanisms of ATP7B-mediated copper export but can also guide the development of therapeutics for the treatment of WD.


Assuntos
Proteínas de Transporte de Cátions , Degeneração Hepatolenticular , Humanos , Proteínas de Transporte de Cátions/genética , Proteínas de Transporte de Cátions/metabolismo , Cobre/metabolismo , Proteínas de Transporte de Cobre , ATPases Transportadoras de Cobre/genética , ATPases Transportadoras de Cobre/metabolismo , Microscopia Crioeletrônica , Degeneração Hepatolenticular/metabolismo
8.
Talanta ; 258: 124398, 2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-36871519

RESUMO

ß-amyloid1-42 (Aß1-42) is a humoral biomarker for early diagnosis of Alzheimer's disease (AD), and exists at a low level in human body. Its sensitive detection is very valuable. The electrochemiluminescence (ECL) assay of Aß1-42 has attracted special attention owing to high sensitivity and simple operation. However, currently reported ECL assays for Aß1-42 usually required the introduction of exogenous coreactants to improve the detection sensitivity. Introducing exogenous coreactants will lead to non-negligible repeatability and stability problems. This work exploited poly [(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-{2,1',3}-thiadazole)] nanoparticles (PFBT NPs) as coreactant-free ECL emitters for detecting Aß1-42. The PFBT NPs, first antibody (Ab1) and antigen Aß1-42 were successively assembled on glassy carbon electrode (GCE). Silica nanoparticles served as a carrier to grow polydopamine (PDA) in situ, and further assembled Au nanoparticles (Au NPs) and second antibody (Ab2), producing the secondary antibody complex (SiO2@PDA-Au NPs-Ab2). With its assembly on the biosensor, the ECL signal decreased since both PDA and Au NPs could quench ECL emission from PFBT NPs. The limit of detection (LOD) of 0.55 fg/mL and limit of quantification (LOQ) of 37.45 fg/mL for Aß1-42 were obtained. PFBT NPs coupling dual-quencher PDA-Au NPs created an excellent ECL system for bioassays, and constructed a sensitive analytical method for Aß1-42.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Humanos , Dióxido de Silício , Peptídeos beta-Amiloides , Ouro , Medições Luminescentes/métodos , Anticorpos , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Limite de Detecção
9.
Proc Natl Acad Sci U S A ; 119(40): e2200835119, 2022 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-36161936

RESUMO

Ice cores from alpine glaciers are unique archives of past global and regional climate conditions. However, recovering climate records from these ice cores is often hindered by the lack of a reliable chronology, especially in the age range of 100 to 500 anni (a) for which radiometric dating has not been available so far. We report on radiometric 39Ar dating of an ice core from the Tibetan Plateau and the construction of a chronology covering the past 1,300 a using the obtained 39Ar ages. This is made possible by advances in the analysis of 39Ar using the laser-based detection method atom trap trace analysis, resulting in a twofold increase in the upper age limit of 39Ar dating. By measuring the anthropogenic 85Kr along with 39Ar we quantify and correct modern air contamination, thus removing a major systematic uncertainty of 39Ar dating. Moreover, the 85Kr data for the top part of the ice core provide information on firn processes, including the age difference between the ice and its enclosed gas. This first application of 39Ar and 85Kr to an ice core facilitates further ice cores from nonpolar glaciers to be used for recovering climate records of the Common Era, a period including pronounced anomalies such as the Little Ice Age and the Medieval Warm Period.


Assuntos
Camada de Gelo , Datação Radiométrica , Clima , Mudança Climática , Datação Radiométrica/métodos , Tibet
10.
Adv Sci (Weinh) ; 9(33): e2203747, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-36117118

RESUMO

Intelligent metasurfaces have gained significant importance in recent years due to their ability to dynamically manipulate electromagnetic (EM) waves. Their multifunctional characteristics, realized by incorporating active elements into the metasurface designs, have huge potential in numerous novel devices and exciting applications. In this article, recent progress in the field of intelligent metasurfaces are reviewed, focusing particularly on tuning mechanisms, hardware designs, and applications. Reconfigurable and programmable metasurfaces, classified as space gradient, time modulated, and space-time modulated metasurfaces, are discussed. Then, reconfigurable intelligent surfaces (RISs) that can alter their wireless environments, and are considered as a promising technology for sixth-generation communication networks, are explored. Next, the recent progress made in simultaneously transmitting and reflecting reconfigurable intelligent surfaces (STAR-RISs) that can achieve full-space EM wave control are summarized. Finally, the perspective on the challenges and future directions of intelligent metasurfaces are presented.

11.
Biosens Bioelectron ; 216: 114629, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36001932

RESUMO

Iridium(III) complexes have been developed as eminent electrochemiluminescence (ECL) luminophores, but their current applications are only limited to anodic ECL emission because of weak cathodic ECL emission. This work explored poly(styrene-co-maleicanhydride) (PSMA) as functional reagent to modulate iridium(III) complexes to simultaneously emit bipolar ECL signals. The prepared iridium(III) nanorods (Ir NRs) were detected strong bipolar ECL emissions at +0.9 V and -2.0 V with N,N-diisopropylethylenediamine (DPEA) and persulfate (S2O82-) as coreactant, respectively. Meanwhile, Ag nanoparticles (Ag NPs) were developed as dual-regulating coreaction accelerator to boost the bipolar emissions of Ir NRs simultaneously. The dual-emitting Ir NRs coupled with dual-regulating coreaction accelerator Ag NPs facilitated the construction of mono-luminophore-based ECL ratio strategy for detecting amyloid-ß oligomers (AßO). When the target AßO appeared, the Mg2+-dependent DNAzyme-powered biped walkers were unlocked to cleave single-stranded S1 immobilized on the surface of magnetic beads (MBs), resulting in the production of massive single-stranded ST. Then, the output ST cleaved hairpin H1 captured by Ir NRs modified electrode to produce numerous single strands, which could initiate the hybridization chain reaction (HCR) between Ag NPs-labeled H2 and Ag NPs-labeled H3 to introduce abundant Ag NPs onto the electrode surface. Due to the enhancement effect of Ag NPs on the bipolar ECL emissions from Ir NRs, the ECL ratio detection of AßO was achieved with the detection limit of 0.62 pM. The unique dual-emitting properties of Ir NRs coupled with dual-regulating effect of Ag NPs provided an interesting mono-luminophore-based ECL ratio sensing platform for biological analysis.


Assuntos
Técnicas Biossensoriais , DNA Catalítico , Nanopartículas Metálicas , Nanotubos , Peptídeos beta-Amiloides , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Irídio , Limite de Detecção , Medições Luminescentes/métodos , Prata , Estirenos
12.
Anal Chem ; 94(23): 8346-8353, 2022 06 14.
Artigo em Inglês | MEDLINE | ID: mdl-35639506

RESUMO

Currently reported polyfluorene-based fluorescence detection usually shows high background signal and low detection sensitivity. This work developed a novel three-dimensional (3D) DNA rolling walker via directional movement on a lipid bilayer (LB) supported by Au@Fe3O4 nanoparticles (NPs) in a polyfluorene-based fluorescence system so that it could achieve significantly improved detection sensitivity and almost zero-background signal detection for miRNA-16. First, the carboxyl-functionalized poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-{2,1',3}-thiadazole)] polymer nanoparticles (c-PFBT PNPs) covalently bonded with amino-labeled single-strand CP and further hybridized with single-strand AP to prepare AP-CP-coupled c-PFBT PNP probes. Meanwhile, Au@Fe3O4 NPs were developed as efficient fluorescence quenchers and served as the matrix for assembling the LB. The resulting Au@Fe3O4@LB assembled cholesterol-labeled orbital DNA L1 and L2 and further assembled hairpins H1 and AP-CP-coupled c-PFBT PNP probes to construct DNA nanomachines. Then, the target miRNA-16 was introduced to initiate the rolling circle amplification (RCA) reaction and form dynamic DNA rolling walkers, thus releasing single-strand CP-coupled c-PFBT PNP probes. The magnetic separation effect of Au@Fe3O4 NPs made it possible to detect the fluorescence signal from the released probes, thus achieving almost zero-background signal detection for miRNA-16 with a low detection limit of 95 aM. The flexible interfaces provided by the LB endowed the DNA rolling walkers with high binding efficiency and low derailment probability, thus achieving significantly improved detection sensitivity. The developed strategy provided an attractive polyfluorene-based fluorescence platform with high-sensitivity and low-background signals.


Assuntos
Técnicas Biossensoriais , MicroRNAs , Nanopartículas , Técnicas Biossensoriais/métodos , DNA , Limite de Detecção , Bicamadas Lipídicas , Técnicas de Amplificação de Ácido Nucleico/métodos , Andadores
13.
Mov Disord ; 37(7): 1531-1535, 2022 07.
Artigo em Inglês | MEDLINE | ID: mdl-35507442

RESUMO

BACKGROUND: Wilson's disease (WD) currently lacks a promising indicator that could reflect neurological impairment and monitor treatment outcome. We aimed to investigate whether serum neurofilament light chain (sNfL) functions as a candidate for disease assessment and treatment monitoring of WD. METHODS: We assessed preclinical and manifested WD patients' sNfL levels compared to controls and analyzed the differences between patients with various clinical symptoms. We then explored the correlation between clinical scales and sNfL levels. And repeated measurements were performed in 34 patients before and after treatment. RESULTS: WD patients with neurological involvement had significantly higher sNfL levels than both hepatic patients and controls. Positive correlations were found between Unified Wilson's Disease Rating Scale scores and sNfL and between semiquantitative magnetic resonance imaging scales and sNfL levels in WD patients. However, in the treatment follow-up analysis, the trend of sNfL before and after treatment disaccorded with clinical response. CONCLUSION: These findings suggest that sNfL levels can be an ideal indicator for the severity of neurological involvement but fail to evaluate change in disease condition after treatment. © 2022 International Parkinson and Movement Disorder Society.


Assuntos
Degeneração Hepatolenticular , Biomarcadores , Degeneração Hepatolenticular/diagnóstico , Degeneração Hepatolenticular/terapia , Humanos , Filamentos Intermediários , Imageamento por Ressonância Magnética , Resultado do Tratamento
14.
Rev Sci Instrum ; 93(2): 023203, 2022 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-35232153

RESUMO

We demonstrate fast analysis of 39Ar/Ar at the 10-16 level using a mass spectrometer for isotope pre-enrichment and an atom trap for counting. An argon gas sample first passes through a dipole mass separator that reduces the dominant isotope 40Ar by two orders of magnitude while preserving both the rare tracer isotope 39Ar and a minor stable isotope 38Ar for control purposes. Measurements of both natural and enriched samples with atom trap trace analysis demonstrate that the 39Ar/38Ar ratios change less than 10%, while the overall count rates of 39Ar are increased by one order of magnitude. By overcoming the analysis-speed bottleneck, this advance will benefit large-scale applications of 39Ar dating in the earth sciences, particularly for mapping ocean circulation.

15.
J Hazard Mater ; 432: 128699, 2022 06 15.
Artigo em Inglês | MEDLINE | ID: mdl-35325864

RESUMO

In general, suitable double luminophores and their coreactants are necessary for constructing electrochemiluminescence (ECL) ratio strategy. However, the complexity of matching double luminophores and the stability and repeatability problem suffered by introducing exogenous coreactant would greatly limit the application of ratio detection. An original single-luminophore-based ECL ratio sensing was developed excluding any exogenous coreactants in this work. The poly [9,9-bis(3'-(N,N-dimethylamino)propyl)- 2,7-fluorene]-alt-2,7-(9,9-dioctylfluorene)] nanoparticles (PFN NPs) were explored to emit two anodic ECL signals. One centered at + 1.25 V (ECL-1) with the scanning potential of 0 ~ + 1.25 V and the other at + 1.95 V (ECL-2) with the scanning potential of 0 ~ + 1.95 V. ECL-1 showed a very strong emission without any exogenous coreactant. Importantly, hydrogen peroxide (H2O2) was able to efficiently weaken ECL-1 but strengthen ECL-2. When organophosphorus pesticides (OPs) were absent, the immobilized acetylcholinesterase-choline oxidase (AChE-ChOx) would catalyze the substrate acetylthiocholine chloride (ATCl) to produce H2O2, resulting in a quenched ECL-1 and an enhanced ECL-2. With the introduction of OPs, ECL-1 increased while ECL-2 accordingly decreased as OPs prohibited production of H2O2 by inhibiting activity of AChE. Highly sensitive ECL ratio detection for OPs was realized based on the change of the ratio of two signals. The dual anode emission properties of PFN NPs coupled with the opposite regulation of H2O2 on the two signals paved a new avenue for potentially tunable ECL ratio sensing strategy, and showed enormous potential applications for OPs analysis.


Assuntos
Técnicas Biossensoriais , Nanopartículas , Praguicidas , Acetilcolinesterase , Técnicas Biossensoriais/métodos , Técnicas Eletroquímicas/métodos , Peróxido de Hidrogênio/química , Medições Luminescentes/métodos , Nanopartículas/química , Compostos Organofosforados , Praguicidas/análise , Polímeros/química
16.
Opt Express ; 29(19): 30579-30589, 2021 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-34614780

RESUMO

This paper presents a new design of linear-polarization metasurface converter with arbitrary polarization rotating angle. The linear-polarization conversion is achieved by first separating the linearly polarized incident wave into two orthogonal circularly polarized waves, then adding an additional phase to one of the circularly polarized waves, and finally recombining these two circularly polarized waves into a linearly polarized wave and reflecting it towards free space. A practical unit cell operating at 10 GHz with sandwich structure is applied to realize the linear-polarization metasurface converter, which consists of a top-layer square patch, a middle-layer ground plane, a bottom-layer 90° quadrature hybrid coupler, and two vias connecting the top layer and bottom layer. The proposed linear-polarization metasurface converter is analyzed theoretically and demonstrated by both simulating and experimental results.

17.
Opt Express ; 29(20): 32031-32041, 2021 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-34615282

RESUMO

We present a time-coding reconfigurable intelligent surface (RIS) enabled spread-spectrum secure wireless communication system. The time-coding spread-spectrum RIS is realized by altering the RIS between the two states of a perfect electrical conductor (PEC) and perfect magnetic conductor (PMC), according to a pseudo-random time sequence, respectively. This spectrum spreading function of the time-coding RIS can be simply applied to the secure wireless communication systems, providing a low-cost, easy-implementation encrypting architecture with the two key features of interception prevention and interference suppression. These two features together with the overall spread-spectrum secure wireless communication system are demonstrated by both theoretical analysis and experimental results using a designed 8 × 8 time-coding RIS.

18.
Rev Sci Instrum ; 92(6): 063204, 2021 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-34243571

RESUMO

Cosmogenic 39Ar dating is an emerging technique in dating mountain glacier ice, mapping ocean circulation, and tracing groundwater flow. We have realized an atom-trap system for the analysis of the radioactive isotope 39Ar (half-life = 269 years) in environmental samples. The system is capable of analyzing small (1-5 kg) environmental water or ice samples and achieves a count rate of 10 atoms/h for 39Ar at the modern isotopic abundance level of 8 × 10-16. By switching frequently between counting 39Ar atoms and measuring the stable and abundant isotope 38Ar, drift effects in the trapping efficiency are largely suppressed, leading to a more precise measurement of the isotope ratio 39Ar/38Ar. Moreover, cleaning techniques are developed to alleviate cross-sample contamination, reducing the background 39Ar count rate down to <0.5 atoms/h. These advances allow us to determine the 39Ar age in the range of 250-1300 years with precisions of <20%.

19.
ACS Appl Mater Interfaces ; 13(27): 32013-32021, 2021 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-34212714

RESUMO

The reported donor donor-acceptor ("DD-A") fluorescence resonance energy transfer (FRET) was typically achieved through random collisions and interactions of DNA molecules in the bulk solution, which has inevitable defects, including weak biological stability, slow reaction kinetics, and low hybridization efficiency. In order to overcome these deficiencies, this work developed a quadrivalent cruciform DNA nanostructure (qCDN)-mediated cascaded catalyzed hairpin assembly (CHA) amplifier for the fluorescence detection of amyloid ß oligomer species (AßOs). First, four H1 and four H2 hairpins were assembled on one qCDN to obtain qCDNH1 and qCDNH2, respectively. In the presence of AßOs, strand C was released from the P1-C hybrid hairpin and then alternately opened qCDNH1 and qCDNH2 to trigger the qCDN-mediated CHA. As a result, double donors in H1 and one acceptor in H2 were mutually closed, and the porous DNA nanonet with a high loading of "DD-A" FRET binary probes was formed. The FRET efficiency was approximately 78%, and the initial reaction rate was 25-fold faster than the conventional CHA. The detection limit of AßOs was as low as 0.69 pM. The combination of the "DD-A" FRET binary probes and qCDN-mediated cascaded amplifier exhibited great promise for detecting biomarkers with trace levels.


Assuntos
Peptídeos beta-Amiloides/química , DNA Cruciforme/química , Transferência Ressonante de Energia de Fluorescência/métodos , Limite de Detecção , Nanoestruturas/química , Multimerização Proteica , Estrutura Quaternária de Proteína
20.
Anal Chem ; 2021 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-34133127

RESUMO

The bifunctional moderator is urgently needed in the field of ratiometric electrochemiluminescence (ECL) sensing since it can mediate simultaneously two ECL signals to conveniently realize their opposite change trend. This work designed a novel dual-signal combined nanoprobe with carboxyl-functionalized poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-{2,1',3}-thiadazole)] nanoparticles (c-PFBT NPs) as the anodic ECL probe and L-cysteine capped CdS quantum dots (L-CdS QDs) as the cathodic ECL probe, which performed a dual-signal output capability without any additional coreactants. More importantly, hydrogen peroxide (H2O2) produced in situ by enzyme-catalyzed reaction was developed as a bifunctional moderator for simultaneously regulating two signals. The dual-signal combined nanoprobe (c-PFBT NPs@CdS QDs) served as the matrix to immobilize acetylcholinesterase (AChE) and choline oxidase for organophosphorus (OPs) analysis. In the absence of OPs, H2O2 was produced by catalyzing the substrate acetylthiocholine (ATCl) with enzymes and it quenched the anodic ECL signal from c-PFBT NPs and simultaneously promoted the cathodic ECL signal from L-CdS QDs. When OPs was present, the activity of AChE was inhibited, the anodic signal would increase, and the cathodic signal would accordingly decrease. The integration of the bifunctional moderator H2O2 and dual-signal combined nanoprobe c-PFBT NPs@CdS QDs not only provides an attractive ECL platform for enzymatic sensing involving the generation or consumption of H2O2 but also paves a new pathway for other ratiometric ECL systems involving enzyme catalytic amplification for detecting antigens, antibodies, DNA, RNA, etc.

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