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1.
Environ Res ; 247: 118215, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38253194

RESUMEN

Identifying sediment phosphorus sources, the key to control eutrophication, is hindered in multi-source polluted urban rivers by the lack of appropriate methods and data resolution. Community-based microbial source tracking (MST) offers new insight, but the bacterial communities could be affected by environmental fluctuations during the migration with sediments, which might induce instability of MST results. Therefore, the effects of environmental-induced community succession on the stability of MST were compared in this study. Liangxi River, a highly eutrophic urban river, was selected as the study area where sediment phosphorus sources are difficult to track because of multi-source pollution and complicated hydrodynamic conditions. Spearman correlation analysis (P < 0.05) was conducted to recognize a close relationship between sediment, bacterial communities and phosphorus, verifying the feasibility of MST for identify sediment phosphorus sources. Two distinct microbial community fingerprints were constructed based on whether excluded 113 vulnerable species, which were identified by analyzing the differences of microorganisms across a concentration gradient of exogenous phosphorus input in microbial environmental response experiment. Because of the lower unknown proportion and relative standard deviations, MST results were more stable and reliable when based on the fingerprints excluding species vulnerable to phosphorus. This study presents a novel insight on how to identify sediment phosphorus sources in multi-source polluted urban river, and would help to develop preferential control strategies for eutrophication management.


Asunto(s)
Microbiota , Contaminantes Químicos del Agua , Ríos , Monitoreo del Ambiente/métodos , Sedimentos Geológicos , Fósforo/análisis , Bacterias , China , Contaminantes Químicos del Agua/toxicidad , Contaminantes Químicos del Agua/análisis
2.
Angew Chem Int Ed Engl ; 63(24): e202404100, 2024 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-38616169

RESUMEN

Exploration of efficient red emitting antimony hybrid halide with large Stokes shift and zero self-absorption is highly desirable due to its enormous potential for applications in solid light emitting, and active optical waveguides. However, it is still challenging and rarely reported. Herein, a series of (TMS)2SbCl5 (TMS=triphenylsulfonium cation) crystals have been prepared with diverse [SbCl5]2- configurations and distinctive emission color. Among them, cubic-phase (TMS)2SbCl5 shows bright red emission with a large Stokes shift of 312 nm. In contrast, monoclinic and orthorhombic (TMS)2SbCl5 crystals deliver efficient yellow and orange emission, respectively. Comprehensive structural investigations reveal that larger Stokes shift and longer-wavelength emission of cubic (TMS)2SbCl5 can be attributed to the larger lattice volume and longer Sb⋅⋅⋅Sb distance, which favor sufficient structural aberration freedom at excited states. Together with robust stability, (TMS)2SbCl5 crystal family has been applied as optical waveguide with ultralow loss coefficient of 3.67 ⋅ 10-4 dB µm-1, and shows superior performance in white-light emission and anti-counterfeiting. In short, our study provides a novel and fundamental perspective to structure-property-application relationship of antimony hybrid halides, which will contribute to future rational design of high-performance emissive metal halides.

3.
Small ; 19(31): e2204158, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-36216592

RESUMEN

It is important to reveal the luminescence mechanisms of carbon dots (CDs). Herein, CDs with two types of optical centers are synthesized from citric acid in formamide by a solvothermal method, and show high photoluminescence quantum yield reaching 42%. Their green/yellow emission exhibits pronounced vibrational structure and high resistance toward photobleaching, while broad red photoluminescence is sensitive to solvents, temperature, and UV-IR. Under UV-IR, the red emission is gradually bleached due to the photoinduced dehydration of the deprotonated surface of CDs in dimethyl sulfoxide, while this process is hindered in water. From the analysis of steady-state and time-resolved photoluminescence and transient absorption data together with density functional theory calculations, the green/ yellow emission is assigned to conjugated sp2 -domains (core state) similar to organic dye derivatives stacked within disk-shaped CDs; and the broad red emission-to oxygen-containing groups bound to sp2 -domains (surface state), whereas energy transfer from the core to the surface state can happen.

4.
Small ; 19(31): e2206667, 2023 08.
Artículo en Inglés | MEDLINE | ID: mdl-36651015

RESUMEN

Obesity is a major global health problem that significantly increases the risk of many other diseases. Herein, a facile method of suppressing lipogenesis and obesity using L-arginine-functionalized carbon dots (L-Arg@CDots) is reported. The prepared CDots with a negative surface charge form stronger bonds than D-arginine and lysine with L-Arg in water. The L-Arg@CDots in the aqueous solution offer a high photoluminescence quantum yield of 23.6% in the red wavelength region. The proposed L-Arg functionalization strategy not only protects the red emission of the CDots from quenching by water molecules but also enhances the intracellular uptake of L-Arg to reduce lipogenesis. Injection of L-Arg@CDots can reduce the body weight increase in ob/ob mice by suppressing their food intake and shrinking the white adipose tissue cells, thereby significantly inhibiting obesity.


Asunto(s)
Carbono , Puntos Cuánticos , Ratones , Animales , Carbono/química , Obesidad , Arginina , Puntos Cuánticos/química
5.
Nat Mater ; 21(8): 896-902, 2022 08.
Artículo en Inglés | MEDLINE | ID: mdl-35835818

RESUMEN

The colour centre platform holds promise for quantum technologies, and hexagonal boron nitride has attracted attention due to the high brightness and stability, optically addressable spin states and wide wavelength coverage discovered in its emitters. However, its application is hindered by the typically random defect distribution and complex mesoscopic environment. Here, employing cathodoluminescence, we demonstrate on-demand activation and control of colour centre emission at the twisted interface of two hexagonal boron nitride flakes. Further, we show that colour centre emission brightness can be enhanced by two orders of magnitude by tuning the twist angle. Additionally, by applying an external voltage, nearly 100% brightness modulation is achieved. Our ab initio GW and GW plus Bethe-Salpeter equation calculations suggest that the emission is correlated to nitrogen vacancies and that a twist-induced moiré potential facilitates electron-hole recombination. This mechanism is further exploited to draw nanoscale colour centre patterns using electron beams.


Asunto(s)
Compuestos de Boro , Color
6.
Opt Express ; 31(10): 16213-16226, 2023 May 08.
Artículo en Inglés | MEDLINE | ID: mdl-37157705

RESUMEN

On the basis of computational ghost imaging (CGI), we present a new imaging technique, feature ghost imaging (FGI), which can convert the color information into distinguishable edge features in retrieved grayscale images. With the edge features extracted by different order operators, FGI can obtain the shape and the color information of objects simultaneously in a single-round detection using one single-pixel detector. The feature distinction of rainbow colors is presented in numerical simulations and the verification of FGI's practical performance is conducted in experiments. Furnishing a new perspective to the imaging of colored objects, our FGI extends the function and the application fields of traditional CGI while sustaining the simplicity of the experimental setup.

7.
Small ; 18(24): e2201694, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35578914

RESUMEN

Inverted perovskite solar cells (PSCs) have received widespread attention due to their facile fabrication and wide applications. However, their power conversion efficiency (PCE) is reported lower than that of regular PSCs because of the undesirable interfacial contact between perovskite and the hydrophobic hole transport layer (HTL). Here, an interface regulation strategy is proposed to overcome this limitation. A small molecule ([2-(9H-carbazol-9-yl) ethyl] phosphonic acid, abbreviated as 2P), composed of carbazole and phosphonic acid groups, is inserted between perovskite and HTL. Morphological characterization and theoretical calculation reveal that perovskite bonds stronger on 2P-modified HTL than on pristine HTL. The improved interfacial contact facilitates hole extraction and retards degradation. Upon the incorporation of 2P, inverted PSCs deliver a high PCE of over 22% with superior stability, keeping 84.6% of initial efficiency after 7200 h storage under an ambient atmosphere with a relative humidity of ≈30-40%. This strategy provides a simple and efficient way to boost the performance of inverted PSCs.

8.
Opt Express ; 30(20): 35923-35936, 2022 Sep 26.
Artículo en Inglés | MEDLINE | ID: mdl-36258532

RESUMEN

Single-pixel imaging (SPI) can perceive the world using only a single-pixel detector, but long sampling times with a series of patterns are inevitable for SPI, which is the bottleneck for its practical application. Developing new patterns to reduce the sampling times might provide opportunities to address this challenge. Based on the Kronecker product of Hadamard matrix, we here design a complete set of new patterns, called Gao-Boole patterns, for SPI. Compared to orthogonal Hadamard basis patterns with elements valued as +1 or -1, our Gao-Boole patterns are non-orthogonal ones and the element values are designed as +1 or 0. Using our Gao-Boole patterns, the reconstructed quality of a target image (N × N pixels) is as high as the Hadamard one but only with half pattern numbers of the Hadamard ones, for both full sampling (N2 for Gao-Boole patterns, 2N2 for Hadamard basis patterns) and undersampling cases in experiment. Effectively reducing the patterns numbers and sampling times without sacrificing imaging quality, our designed Gao-Boole patterns provide a superior option for structural patterns in SPI and help to steer SPI toward practical imaging application.

9.
Small ; 17(43): e2100809, 2021 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-34121324

RESUMEN

Hybrid halide perovskites emerging as a highly promising class of functional materials for semiconductor optoelectronic applications have drawn great attention from worldwide researchers. In the past few years, prominent nonlinear optical properties have been demonstrated in perovskite bulk structures indicating their bright prospect in the field of nonlinear optics (NLO). Following the surge of 3D perovskites, more recently, the low-dimensional perovskites (LDPs) materials ranging from two-, one-, to zero-dimension such as quantum-wells or colloidal nanostructures have displayed unexpectedly attractive NLO response due to the strong quantum confinement, remarkable exciton effect, and structural diversity. In this perspective, the current state of the art is reviewed in the field of NLO for LDP materials. The relationship between confinement effect and NLO is analyzed systematically to give a comprehensive understanding of the function of dimension reduction. Furthermore, future directions and challenges toward the improvement of the NLO in LDP materials are discussed to provide an outlook in this rapidly developing field.

10.
Small ; 17(43): e2101359, 2021 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-34121319

RESUMEN

Colloidal all-inorganic perovskites nanocrystals (NCs) have emerged as a promising material for display and lighting due to their excellent optical properties. However, blue emissive NCs usually suffer from low photoluminescence quantum yields (PLQYs) and poor stability, rendering them the bottleneck for full-color all-perovskite optoelectronic applications. Herein, a facile approach is reported to enhance the emission efficiency and stability of blue emissive perovskite nano-structures via surface passivation with potassium bromide. By adding potassium oleate and excess PbBr2 to the perovskite precursor solutions, potassium bromide-passivated (KBr-passivated) blue-emitting (≈450 nm) CsPbBr3 nanoplatelets (NPLs) is successfully synthesized with a respectably high PLQY of 87%. In sharp contrast to most reported perovskite NPLs, no shifting in emission wavelength is observed in these passivated NPLs even after prolonged exposures to intense irradiations and elevated temperature, clearly revealing their excellent photo- and thermal-stabilities. The enhancements are attributed to the formation of K-Br bonding on the surface which suppresses ion migration and formation of Br-vacancies, thus improving both the PL emission and stability of CsPbBr3 NPLs. Furthermore, all-perovskite white light-emitting diodes (WLEDs) are successfully constructed, suggesting that the proposed KBr-passivated strategy can promote the development of the perovskite family for a wider range of optoelectronic applications.

11.
Nanotechnology ; 31(48): 485207, 2020 Nov 27.
Artículo en Inglés | MEDLINE | ID: mdl-32931471

RESUMEN

1D ZnO nanostructures have been widely explored due to their potential applications in ultraviolet (UV) region photodetectors because of their unique structural and optoelectronic properties. However, a large number of surface defect states leading to a noticeable dark current hinders their practical applications in UV photodetection. In this work, we have shown improved ZnO/Al2O3 core-shell microrod photodetectors, whose performance is significantly enhanced by defect passivation and the introduction of trap states by atomic layer deposition grown thin amorphous Al2O3 shell layer, as evidenced by steady-state and transient photoluminescence investigations. The photodetectors demonstrated suppressed dark current and increased photocurrent after capping the Al2O3 layer. Specifically, the ZnO/Al2O3 core-shell microrod photodetector exhibited a photoresponsivity as high as 0.019 A/(W cm-2) with the dark current as low as ∼1 × 10-11 A, and a high I light/I dark ratio of ∼104 under relatively weak light illumination (∼10 µW cm-2). The results presented in this work provide valuable pathways to boost the performance of 1D ZnO microrod-based photodetectors for future practical applications.

12.
Angew Chem Int Ed Engl ; 59(49): 22156-22162, 2020 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-32803819

RESUMEN

Quasi-two-dimensional (2D) perovskites are promising candidates for light generation owing to their high radiative rates. However, strong exciton-phonon interactions caused by mechanical softening of the surface act as a bottleneck in improving their suitability for a wide range of lighting and display applications. Moreover, it is not easily available to tune the phonon interactions in bulk films. Here, we adopt bottom-up fabricated blue emissive perovskite nanoplatelets (NPLs) as model systems to elucidate and as well as tune the phonon interactions via engineering of binary NPL solids. By optimizing component domains, the phonon coupling strength can be reduced by a factor of 2 driven by the delocalization of 2D excitons in out-of-plane orientations. It shows the picosecond energy transfer originated from the Förster resonance energy transfer (FRET) efficiently competes with the exciton-phonon interactions in the binary system.

13.
Small ; 15(50): e1905050, 2019 12.
Artículo en Inglés | MEDLINE | ID: mdl-31721434

RESUMEN

Upconversion near-infrared (NIR) fluorescent carbon dots (CDs) are important for imaging applications. Herein, thermally activated upconversion photoluminescence (UCPL) in the NIR region, with an emission peak at 784 nm, which appears under 808 nm continuous-wave laser excitation, are realized in the NIR absorbing/emissive CDs (NIR-CDs). The NIR-CDs are synthesized by microwave-assisted exfoliation of red emissive CDs in dimethylformamide, and feature single or few-layered graphene-like cores. This structure provides an enhanced contact area of the graphene-like plates in the core with the electron-acceptor carbonyl groups in dimethylformamide, which contributes to the main NIR absorption band peaked at 724 nm and a tail band in 800-850 nm. Temperature-dependent photoluminescence spectra and transient absorption spectra confirm that the UCPL of NIR-CDs is due to the thermally activated electron transitions in the excited state, rather than the multiphoton absorption process. Temperature dependent upconversion NIR luminescence imaging is demonstrated for NIR-CDs embedded in a polyvinyl pyrrolidone film, and the NIR upconversion luminescence imaging in vivo using NIR-CDs in a mouse model is accomplished.


Asunto(s)
Carbono/química , Rayos Infrarrojos , Luminiscencia , Microondas , Puntos Cuánticos/química , Temperatura , Animales , Ratones , Tamaño de la Partícula , Espectroscopía de Fotoelectrones , Puntos Cuánticos/ultraestructura , Difracción de Rayos X
14.
Opt Express ; 26(13): 17511-17518, 2018 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-30119562

RESUMEN

Compared with conventional lasers, the random laser is realized through strong multiple scatterings in disordered gain system. In this paper, random lasing (RL) in one-dimensional metal surface plasmon (SP) waveguide with gold-plated self-formed silicon pyramids was investigated comprehensively. Consequently, the emission intensity of RL was enhanced dramatically and the RL threshold was reduced significantly through Au-coated Si spiky tips. Meanwhile, one-dimensional metal SP channel waveguides confined the emitting light in a certain direction with a small divergence angle. Using FDTD simulations, it was found that the enhancement effect for RL is likely attributed to the localized surface plasmon (LSP) field. In addition, the LSP field nearby the spiky tips can enhance field-molecule interaction, which was benefit for lasing in small scale. The results in this letter supplied a feasible method to realize the application of RL in subwavelength optical elements.

15.
Angew Chem Int Ed Engl ; 57(32): 10236-10240, 2018 Aug 06.
Artículo en Inglés | MEDLINE | ID: mdl-29943501

RESUMEN

Understanding the interactions between a semiconducting nanocrystal surface and chiral anchoring molecules could resolve the mechanism of chirality induction in nanoscale and facilitate the rational design of chiral semiconducting materials for chiroptics. Now, chiral molybdenum oxide nanoparticles are presented in which chirality is transferred via a bio-to-nano approach. With facile control of the amount of chiral cysteine molecules under redox treatment, circular dichroism (CD) signals are generated in the plasmon region and metal-ligand charge-transfer band. The obtained enhanced CD signals with tunable lineshapes illustrate the possibility of using chiral molybdenum oxide nanoparticles as potentials for chiral semiconductor nanosensors, optoelectronics, and photocatalysts.

16.
Small ; 13(44)2017 11.
Artículo en Inglés | MEDLINE | ID: mdl-28961373

RESUMEN

Pressure sensing is a crucial function for flexible and wearable electronics, such as artificial skin and health monitoring. Recent progress in material and device structure of pressure sensors has brought breakthroughs in flexibility, self-healing, and sensitivity. However, the fabrication process of many pressure sensors is too complicated and difficult to integrate with traditional silicon-based Micro-Electro-Mechanical System(MEMS). Here, this study demonstrates a scalable and integratable contact resistance-based pressure sensor based on a carbon nanotube conductive network and a photoresist insulation layer. The pressure sensors have high sensitivity (95.5 kPa-1 ), low sensing threshold (16 Pa), fast response speed (<16 ms), and zero power consumption when without loading pressure. The sensitivity, sensing threshold, and dynamic range are all tunable by conveniently modifying the hole diameter and thickness of insulation layer.

18.
Phys Chem Chem Phys ; 18(29): 19631-6, 2016 Jul 20.
Artículo en Inglés | MEDLINE | ID: mdl-27381840

RESUMEN

The band gap width of the Be-doped ZnO correlates strongly with the distribution of the dopants. By performing first-principles calculations, it is found that an interstitial Be (Bei) atom preferably migrates in a basal plane. During the migration, such a Bei atom favorably bonds to a substituted Be (BeZn) atom, forming a new defect complex (2Be)Zn, showing a trend of aggregation of Be atoms in ZnO. Furthermore, the stability of the defect complex (2Be)Zn can be weakened by a substituted Mg (MgZn). So, the Mg impurities in Be-doped ZnO might suppress the aggregation of Be, so as to significantly improve the effect of the doped Be on modulating the band gap of ZnO.

19.
J Colloid Interface Sci ; 668: 132-141, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38669991

RESUMEN

A key challenge to enhance the therapeutic outcome of photothermal therapy (PTT) is to improve the efficiency of passive targeted accumulation of photothermal agents at tumor sites. Carbon dots (CDs) are an ideal choice for application as photothermal agents because of their advantages such as adjustable fluorescence, high photothermal conversion efficiency, and excellent biocompatibility. Here, we synthesized polylysine-modified near-infrared (NIR)-emitting CDs assemblies (plys-CDs) through post-solvothermal reaction of NIR-emitting CDs with polylysine. The encapsulated structure of plys-CDs was confirmed by determining morphological, chemical, and luminescent properties. The particle size of CDs increased to approximately 40 ± 8 nm after polylysine modification and was within the size range appropriate for achieving superior enhanced permeability and retention effect. Plys-CDs maintained a high photothermal conversion efficiency of 54.9 %, coupled with increased tumor site accumulation, leading to a high efficacy in tumor PTT. Thus, plys-CDs have a great potential for application in photothermal ablation therapy of tumors.


Asunto(s)
Carbono , Rayos Infrarrojos , Tamaño de la Partícula , Terapia Fototérmica , Polilisina , Puntos Cuánticos , Polilisina/química , Carbono/química , Animales , Puntos Cuánticos/química , Ratones , Humanos , Ratones Endogámicos BALB C , Propiedades de Superficie , Femenino , Supervivencia Celular/efectos de los fármacos , Neoplasias/terapia , Neoplasias/patología
20.
Chemistry ; 19(30): 9818-24, 2013 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-23788127

RESUMEN

As some of the most interesting metal-free catalysts, carbon nanotubes (CNTs) and other carbon-based nanomaterials show great promise for some important chemical reactions, such as the selective oxidation of cyclohexane (C6H12). Due to the lack of fundamental understanding of carbon catalysis in liquid-phase reactions, we have sought to unravel the role of CNTs in the catalytic oxidation of C6H12 through a combination of kinetic analysis, in situ spectroscopy, and density functional theory. The catalytic effect of CNTs originates from a weak interaction between radicals and their graphene skeletons, which confines the radicals around their surfaces. This, in turn, enhances the electron-transfer catalysis of peroxides to yield the corresponding alcohol and ketone.

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