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1.
Adv Mater ; : e2312004, 2024 Feb 24.
Artículo en Inglés | MEDLINE | ID: mdl-38402422

RESUMEN

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral 1D edge states. Yet, in magnetic topological insulators to date, topological protection is far from robust, with zero-magnetic field QAH effect only realized at temperatures an order of magnitude below the Néel temperature TN , though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realizing QAH effect at higher temperatures. Here a scanning tunneling microscope is used to directly map the size of exchange gap (Eg,ex ) and its spatial fluctuation in the QAH insulator 5-layer MnBi2 Te4 . Long-range fluctuations of Eg,ex are observed, with values ranging between 0 (gapless) and 70 meV, appearing to be uncorrelated to individual surface point defects. The breakdown of topological protection is directly imaged, showing that the gapless edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless regions in the bulk. Finally, it is unambiguously demonstrated that the gapless regions originate from magnetic disorder, by demonstrating that a small magnetic field restores Eg,ex in these regions, explaining the recovery of topological protection in magnetic fields. The results indicate that overcoming magnetic disorder is the key to exploiting the unique properties of QAH insulators.

2.
Analyst ; 148(24): 6223-6227, 2023 Dec 04.
Artículo en Inglés | MEDLINE | ID: mdl-37942940

RESUMEN

We propose a novel ligand-assisted reprecipitation method to synthesize aqueous-phase CsPbBr3 nanocrystals, the fluorescence intensity of which remained at 51% after 120 h. As a multifunctional additive, cesium trifluoroacetate (Cs-TFA) can improve the surface adsorption energy and induce nanocrystals to show significant anodic electrochemiluminescence (ECL) and stable cathodic ECL performances.

3.
ACS Nano ; 17(16): 15441-15448, 2023 Aug 22.
Artículo en Inglés | MEDLINE | ID: mdl-37552585

RESUMEN

Emergent quantum phenomena in two-dimensional van der Waal (vdW) magnets are largely governed by the interplay between exchange and Coulomb interactions. The ability to precisely tune the Coulomb interaction enables the control of spin-correlated flat-band states, band gap, and unconventional magnetism in such strongly correlated materials. Here, we demonstrate a gate-tunable renormalization of spin-correlated flat-band states and bandgap in magnetic chromium tribromide (CrBr3) monolayers grown on graphene. Our gate-dependent scanning tunneling spectroscopy (STS) studies reveal that the interflat-band spacing and bandgap of CrBr3 can be continuously tuned by 120 and 240 meV, respectively, via electrostatic injection of carriers into the hybrid CrBr3/graphene system. This can be attributed to the self-screening of CrBr3 arising from the gate-induced carriers injected into CrBr3, which dominates over the weakened remote screening of the graphene substrate due to the decreased carrier density in graphene. Precise tuning of the spin-correlated flat-band states and bandgap in 2D magnets via electrostatic modulation of Coulomb interactions not only provides effective strategies for optimizing the spin transport channels but also may exert a crucial influence on the exchange energy and spin-wave gap, which could raise the critical temperature for magnetic order.

4.
Langmuir ; 38(40): 12390-12398, 2022 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-36179217

RESUMEN

g-C3N4-assisted interface engineering has been developed as an effective method to improve the efficiency and stability of perovskite solar cells (PSCs). However, most of the reported works used g-C3N4-induced single-interface modification, which is difficult to passivate the bilateral interfaces of the perovskite layer at the same time. In this paper, we fabricated two kinds of C3N4 materials simultaneously (w-CN and y-CN) after the twice calcination of melamine and used them in the bilateral interface modification toward all-inorganic PSCs. The two kinds of C3N4 play different roles in different interface engineering. On the front interface, w-CN could optimize band level arrangement and improve the perovskite film quality, which contributes to the efficiency of the device. On the back interface, y-CN could also improve the film quality of the perovskite layer, accelerating the extraction of charge carriers. The champion efficiency of the CsPbIBr2-based device treated by the bilateral interface is significantly enhanced from 7.8 to 10.1%. Moreover, the modified perovskite film exhibits negligible degradation after 40 min of exposure in the ambient environment with a relative humidity of 70%, while the pristine perovskite film has a rapid degradation within 20 min.

5.
Mikrochim Acta ; 189(6): 241, 2022 06 01.
Artículo en Inglés | MEDLINE | ID: mdl-35648245

RESUMEN

A novel deep-ultraviolet and dual-emission carbon nanodots (DUCDs)-based dual-channel ratiometric probe was prepared by a one-pot environmental-friendly hydrothermal process using guanidine as the only starting material for sensing polyphenol in tea sample (TPPs). Under the exposure to TPPs, the DUCDs not only provided a characteristic colorimetric response to TPPs, but also displayed TPPs-sensitive ratiometric fluorescence quenching. The detection mechanism was proved to be that enrichment-specific hydroxyl sites (e.g., -NH2 and -COOH) of DUCDs can specifically react with phenolic hydroxyl groups of TPPs to generate dynamic amide and carboxylate bonds by dehydration and/or condensation reaction. As a result, a new carbon nanomaterial with decrement of surface passivation groups, inherent light-absorbing, and invalid fluorescence emission was generated. The ratio (FL297nm/FL395nm) of fluorescence intensity at 297 nm and 395 nm of DUCDs excited at 275 nm decreased with increasing TPPs concentration. The linearity range was 5.0 ng/mL to 100 µg/mL with a detection limit (DL) of 3.5 ± 0.04 ng/mL for TPPs (n = 3, 3σ/k). Colorimetry of DUCDs, best measured as absorbance at 320 nm, was increased linearly in the TPP concentration range 200 ng/mL-200 µg/mL with a DL of 94.7 ± 0.04 ng/mL (n = 3, 3σ/k). The probe was successfully applied to the determination of TPPs in real tea samples, showing potential application prospects in food analysis.


Asunto(s)
Carbono , Puntos Cuánticos , Carbono/química , Colorantes Fluorescentes/química , Polifenoles , Puntos Cuánticos/química ,
6.
Adv Mater ; 34(21): e2107520, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35261089

RESUMEN

Combining magnetism and nontrivial band topology gives rise to quantum anomalous Hall (QAH) insulators and exotic quantum phases such as the QAH effect where current flows without dissipation along quantized edge states. Inducing magnetic order in topological insulators via proximity to a magnetic material offers a promising pathway toward achieving the QAH effect at a high temperature for lossless transport applications. One promising architecture involves a sandwich structure comprising two single-septuple layers (1SL) of MnBi2 Te4 (a 2D ferromagnetic insulator) with ultrathin few quintuple layer (QL) Bi2 Te3 in the middle, and it is predicted to yield a robust QAH insulator phase with a large bandgap greater than 50 meV. Here, the growth of a 1SL MnBi2 Te4 /4QL Bi2 Te3 /1SL MnBi2 Te4 heterostructure via molecular beam epitaxy is demonstrated and the electronic structure probed using angle-resolved photoelectron spectroscopy. Strong hexagonally warped massive Dirac fermions and a bandgap of 75 ± 15 meV are observed. The magnetic origin of the gap is confirmed by the observation of the exchange-Rashba effect, as well as the vanishing bandgap above the Curie temperature, in agreement with density functional theory calculations. These findings provide insights into magnetic proximity effects in topological insulators and reveal a promising platform for realizing the QAH effect at elevated temperatures.

7.
ACS Appl Mater Interfaces ; 14(4): 6102-6108, 2022 Feb 02.
Artículo en Inglés | MEDLINE | ID: mdl-35050569

RESUMEN

Understanding the air stability of MnBi2Te4 thin films is crucial for the development and long-term operation of electronic devices based on magnetic topological insulators. In the present work, we study MnBi2Te4 thin films upon exposure to the atmosphere using a combination of synchrotron-based photoelectron spectroscopy, room-temperature electrical transport, and atomic force microscopy to determine the oxidation process. After 2 days of air exposure, a 2 nm thick oxide passivates the surface, corresponding to the oxidation of only the top two surface layers, with the underlying layers preserved. This protective oxide layer results in samples that still exhibit metallic conduction even after several days of air exposure. Furthermore, the work function decreases from 4.4 eV for pristine MnBi2Te4 to 4.0 eV after the formation of the oxide, along with only a small shift in the core levels, indicating minimal doping as a result of air exposure. With the oxide confined to the top surface layers, and the underlying layers preserved, it may be possible to explore new avenues in how to handle, prepare, and passivate future MnBi2Te4 devices.

8.
Biosensors (Basel) ; 13(1)2022 Dec 30.
Artículo en Inglés | MEDLINE | ID: mdl-36671893

RESUMEN

In this study, we proposed a novel Ru(bpy)32+-Au-WS2 nanocomposite (Ru-Au-WS2 NCs) nano-hybrid electrochemiluminescence (ECL) probe for the highly sensitive detection of carcinoembryonic antigen (CEA). This system utilizes Au nanoparticles (Au NPs) as a bridge to graft the high-performance of a Ru(bpy)32+ ECL emitter and WS2 nanosheet with excellent electrochemical performance into an ECL platform, which shows outstanding anodic ECL performance and biosensing platform due to the synergetic effect and biocompatibility of Au NPs and WS2 nanosheet. Because the ECL intensity of Ru(bpy)32+ is sensitively affected by the antibody-antigen insulator, a preferable linear dependence was obtained in the concentration range of CEA from 1 pg·mL-1 to 350 ng·mL-1 with high selectivity (LOD of 0.3 pg·mL-1, S/N = 3). Moreover, the ECL platform had good reproducibility and stability and exhibited excellent anti-interference performance in the detection process of CEA. We believe that the platform we have developed can expand the opportunities for the detection of additional high specificity-related antibodies/antigens and demonstrate broad prospects for disease diagnosis and biochemical research.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Antígeno Carcinoembrionario , Oro , Reproducibilidad de los Resultados , Técnicas Electroquímicas , Mediciones Luminiscentes , Inmunoensayo , Límite de Detección
9.
ACS Nano ; 15(8): 13444-13452, 2021 Aug 24.
Artículo en Inglés | MEDLINE | ID: mdl-34387086

RESUMEN

Intrinsic magnetic topological insulators offer low disorder and large magnetic band gaps for robust magnetic topological phases operating at higher temperatures. By controlling the layer thickness, emergent phenomena such as the quantum anomalous Hall (QAH) effect and axion insulator phases have been realized. These observations occur at temperatures significantly lower than the Néel temperature of bulk MnBi2Te4, and measurement of the magnetic energy gap at the Dirac point in ultrathin MnBi2Te4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement of the layer-dependent energy gap and verification of a temperature-dependent topological phase transition from a large band gap QAH insulator to a gapless TI paramagnetic phase. Here we utilize temperature-dependent angle-resolved photoemission spectroscopy to study epitaxial ultrathin MnBi2Te4. We directly observe a layer-dependent crossover from a 2D ferromagnetic insulator with a band gap greater than 780 meV in one septuple layer (1 SL) to a QAH insulator with a large energy gap (>70 meV) at 8 K in 3 and 5 SL MnBi2Te4. The QAH gap is confirmed to be magnetic in origin, as it becomes gapless with increasing temperature above 8 K.

10.
Analyst ; 146(14): 4566-4575, 2021 Jul 12.
Artículo en Inglés | MEDLINE | ID: mdl-34152330

RESUMEN

p-Nitrophenol and its derivatives can cause serious harm to the health of mankind and the earth's ecosystem. Therefore, it is necessary to develop a novel and rapid detection technology for p-nitrophenol and its derivative. Herein, excellent water-soluble, large-size and dual-emissive neuron cell-analogous carbon-based probes (NCNPs) have been prepared via a solvothermal approach, using o-phenylenediamine as the only precursor, which exhibit two distinctive fluorescence (FL) peaks at 420 and 555 nm under 345 nm excitation. The NCNPs show a neuron cell-like branched structure, are cross-connected, and are in the range of 10-20 nm in skeleton diameter. Interestingly, their blue-green dual-colour fluorescence is quenched by p-nitrophenol or its derivative due to the specific mechanism of the ππ stacking interactions or internal filtration effect. Accordingly, a simple, rapid, direct and free-label ratiometric FL detection of p-nitrophenol is proposed. An excellent linear relationship shows linear regions over the range of 0.1-50 µM between the ratio of the FL intensity (FL555 nm/FL420 nm) and the concentrations of p-nitrophenol. The detection limit is as low as 43 nM (3σ). Importantly, the NCNP-based probe also shows acceptable repeatability and reproducibility for the detection of p-nitrophenol and its derivatives, and the recovery results for p-nitrophenol in real wastewater samples are favourable.


Asunto(s)
Puntos Cuánticos , Ecosistema , Colorantes Fluorescentes , Neuronas , Nitrofenoles , Reproducibilidad de los Resultados
11.
ACS Omega ; 5(10): 5407-5411, 2020 Mar 17.
Artículo en Inglés | MEDLINE | ID: mdl-32201831

RESUMEN

In this study, we report a metal-ion-assisted precipitation etching strategy that can be used to manipulate the optical properties associated with the assembling of sulfur quantum dots (S dots) using copper ions. Transmission electron microscopy confirmed that the S dots were mainly distributed within 50-80 nm and that they exhibited an ambiguous boundary. After the post-synthetic Cu2+-assisted modification was completed, the assisted precipitation-etching S dots (APE-S dots) were observed to exhibit a relatively clear boundary with a high fluorescence (FL) quantum yield (QY) of 32.8%. Simultaneously, the Fourier transform infrared radiation, X-ray photoelectron spectra, and time-resolved FL decay spectra were used to illustrate the improvement in the FL QY of the APE-S dots.

12.
Chem Commun (Camb) ; 52(83): 12342-12345, 2016 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-27709162

RESUMEN

This study reports a host-guest interaction strategy for systematically manipulating the optical properties of cesium lead halide perovskite nanocrystals (CsPbBr3 NCs) by protectant-mediated mercapto-ß-cyclodextrin (SH-ß-CD). The fluorescence of CsPbBr3 NCs can be adjusted over 405-510 nm with the quantum yields (QY) maintained at 50-90%.

13.
Analyst ; 139(7): 1751-5, 2014 Apr 07.
Artículo en Inglés | MEDLINE | ID: mdl-24496079

RESUMEN

This work presents the enhanced electrochemiluminescence (ECL) of a newly prepared nanosilver-carbon nanodot (Ag-C-dot) composite and its application for the sensitive detection of sulfide (S(2-)) ions. The Ag-C-dot composite was easily prepared by adding silver nitrate into C-dot colloids through an alkaline reduction. The obtained Ag-C-dots were characterized by UV-vis spectra, fluorescence spectra and transmission electron microscopy. The electrochemical and ECL behaviors of the Ag-C-dot composite were investigated by cyclic voltammetry. Moreover, a simple label-free method to detect S(2-) ions with a high selectivity and sensitivity has been developed based on the ECL of the Ag-C-dot composite in aqueous media. The sensing mechanism could be due to the strong and specific interaction between the S(2-) ions and the Ag atoms/ions on the surface of the Ag-C-dot composite, which dramatically affects the resulting ECL of the Ag-C-dot composite. The linear response to detect S(2-) ions ranges from 0.05 to 100 µM with a detection limit of 0.027 µM (~1 ppb). This work indicates that the Ag-C-dot nanocomposite possesses potential applications for environment sensing.

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