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1.
Nat Commun ; 15(1): 9509, 2024 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-39496620

RESUMO

A promising route towards the deterministic creation and annihilation of single-phonons is to couple a single-photon emitter to a mechanical resonator. The challenge lies in reaching the resolved-sideband regime with a large coupling rate and a high mechanical quality factor. We achieve this by coupling self-assembled InAs quantum dots to a small mode-volume phononic-crystal resonator with mechanical frequency Ωm/2π = 1.466 GHz and quality factor Qm = 2.1 × 103. Thanks to the high coupling rate of gep/2π = 2.9 MHz, and by exploiting a matching condition between the effective Rabi and mechanical frequencies, we observe the interaction between the two systems via correlations in the emitted photons. Our results represent a major step towards quantum control of the mechanical resonator via a single-photon emitter.

2.
Cancer Manag Res ; 16: 1405-1416, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-39411686

RESUMO

Purpose: DNA methylation plays a regulatory role in the oncogenesis and tumor progression and is valuable in the diagnosis and prognosis of cancer. While circulating tumor DNA (ctDNA) is widely used in the detection of oncogenic mutations and the guidance of treatment in advanced non-small cell lung cancer (NSCLC), studies of ctDNA methylation remains insufficient. We aim to investigate the methylation profiles of ctDNA in patients with advanced NSCLC undergoing EGFR-tyrosine kinase inhibitor (EGFR-TKI) therapy and to discover novel biomarkers with predictive or prognostic value. Patients and Methods: We recruited 49 patients with EGFR-mutated advanced NSCLC undergoing EGFR-TKI as first-line treatment. Utilizing next-generation sequencing, we examined the somatic mutations and methylation signatures within the tumor-associated genomic regions of ctDNA from pre-treatment blood. Subsequently, we explored the association of these molecular features with the patients' response to therapy and their progression-free survival (PFS). Results: Genomic mutation profiling revealed no significant association of PFS or best overall response (BOR) and ctDNA status. Evaluation of ctDNA methylation showed a negative correlation between the methylation of small nucleolar RNA (snoRNA) genes and PFS (R=-0.31, P=0.043). Furthermore, high-level methylation of SNORD3F was associated with poorer PFS (mPFS 346d vs 243d, HR 0.49, 95% CI 0.24-0.93, P=0.029). Conclusion: Our study explored the prognostic value of ctDNA methylation in patients with advanced NSCLC undergoing targeted therapies and first revealed the predictive role of SNORD3F.

3.
Angew Chem Int Ed Engl ; : e202409006, 2024 Jun 19.
Artigo em Alemão | MEDLINE | ID: mdl-38896505

RESUMO

Fluoroalkyl-grafted polyoxometalate nanoclusters are used as supramolecular additives to precisely modify the ionic domains of Nafion, which can increase the proton conductivity and selectivity simultaneously. The resulting hybrid membranes show significantly enhanced power density in fuel cells and improved energy efficiency in vanadium flow batteries.

4.
Org Biomol Chem ; 22(20): 4179-4189, 2024 05 22.
Artigo em Inglês | MEDLINE | ID: mdl-38716654

RESUMO

Aspergillus versicolor, an endophytic fungus associated with the herbal medicine Pedicularis sylvatica, produced four new polyketides, aspeversins A-D (1-2 and 5-6) and four known compounds, O-methylaverufin (2), aversin (3), varilactone A (7) and spirosorbicillinol A (8). Their structures were elucidated by extensive spectroscopic data analysis, and their absolute configurations were determined by calculated electronic circular dichroism (ECD) and Mo2(AcO)4-induced CD data. Compound 5 was found to exhibit α-glucosidase inhibitory activity with an IC50 value of 25.57 µM. An enzyme kinetic study indicated that 5 was a typical uncompetitive inhibitor toward α-glucosidase, which was supported by a molecular docking study. Moreover, compounds 1-3 and 5 also improved the cell viability of PC12 cells on a 1-methyl-4-phenylpyridinium (MPP+)-induced Parkinson's disease model, indicating their neuroprotective potential as antiparkinsonian agents.


Assuntos
Aspergillus , Inibidores de Glicosídeo Hidrolases , Fármacos Neuroprotetores , Policetídeos , alfa-Glucosidases , Animais , Ratos , alfa-Glucosidases/metabolismo , Aspergillus/química , Sobrevivência Celular/efeitos dos fármacos , Inibidores de Glicosídeo Hidrolases/farmacologia , Inibidores de Glicosídeo Hidrolases/química , Inibidores de Glicosídeo Hidrolases/isolamento & purificação , Simulação de Acoplamento Molecular , Estrutura Molecular , Fármacos Neuroprotetores/farmacologia , Fármacos Neuroprotetores/química , Fármacos Neuroprotetores/isolamento & purificação , Células PC12 , Policetídeos/farmacologia , Policetídeos/química , Policetídeos/isolamento & purificação
5.
Environ Res ; 248: 117809, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38072114

RESUMO

Formulating suitable policies is essential for resources and environmental management. In this study, an agricultural pollutants emission trading management model driven by water resources and pollutants control is developed to search reasonable policies for agricultural water resources allocation under multiple uncertainties. Random-fuzzy and interval information in water resources system that have directly impact on the effectiveness of management schemes is reflected through interval two-stage stochastic fuzzy-probability programming. The model was root from regional agricultural water resources system in Jining City, China under considering the relationship among effective precipitation, crop water demand, and pollutants emission. Two types policies (water consumption-control and pollutants emission-control) are designed for searching the related interaction on water resources management and water quality improvement. The results indicated that water resources policies would be of water and environmental double benefits, and a large rainfall would reduce irrigation amount from water sources and lead to a larger pollutants emission trading. The results will help for defining scientific and effective water resources protection and management policies and analyzing the related interacted effects on water consumption, pollutants control and system benefit.


Assuntos
Agricultura , Lógica Fuzzy , Incerteza , Probabilidade , Agricultura/métodos , Qualidade da Água , Recursos Hídricos , China , Modelos Teóricos
6.
Phys Rev Lett ; 131(21): 210805, 2023 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-38072607

RESUMO

A spin-photon interface should operate with both coherent photons and a coherent spin to enable cluster-state generation and entanglement distribution. In high-quality devices, self-assembled GaAs quantum dots are near-perfect emitters of on-demand coherent photons. However, the spin rapidly decoheres via the magnetic noise arising from the host nuclei. Here, we address this drawback by implementing an all-optical nuclear-spin cooling scheme on a GaAs quantum dot. The electron-spin coherence time increases 156-fold from T_{2}^{*}=3.9 ns to 0.608 µs. The cooling scheme depends on a non-collinear term in the hyperfine interaction. The results show that such a term is present even though the strain is low and no external stress is applied. Our work highlights the potential of optically active GaAs quantum dots as fast, highly coherent spin-photon interfaces.

7.
Nano Lett ; 23(22): 10414-10422, 2023 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-37930644

RESUMO

Ion-conducting membranes (ICMs) with high selectivity are important components in redox flow batteries. However it is still a challenge to break the trade-off between ion conductivity and ion selectivity, which can be resolved by the regulation of their nanostructures. Here, polyoxometalate (POM)-hybridized block copolymers (BCPs) are used as self-assembled additives to construct proton-selective nanobarriers in the ICM matrix to improve the microscopic structures and macroscopic properties of ICMs. Benefiting from the co-assembly behavior of BCPs and POMs and their cooperative noncovalent interactions with the polymer matrix, ∼50 nm ellipsoidal functional nanoassemblies with hydrophobic vanadium-shielding cores and hydrophilic proton-conducting shells are constructed in the sulfonated poly(ether ether ketone) matrix, which leads to an overall enhancement of proton conductivity, proton selectivity, and cell performance. These results present a self-assembly route to construct functional nanostructures for the modification of polymer electrolyte membranes toward emerging energy technologies.

8.
Sci Rep ; 13(1): 12488, 2023 08 01.
Artigo em Inglês | MEDLINE | ID: mdl-37528182

RESUMO

A systematic understanding of the spatio-temporal changes and driving factors in the Qinghai-Tibet Plateau holds significant scientific reference value for the future of ecological sustainable development. This paper utilizes MODIS normalized difference vegetation index (NDVI) and meteorological data to investigate the spatio-temporal changes and driving factors of vegetation coverage in the Qinghai-Tibet Plateau from 2001 to 2020. Methods employed include the dimidiate pixel model, trend analysis, partial correlation analysis, and residual analysis. The results demonstrate a generally fluctuating upward trend in vegetation coverage across the Tibetan Plateau over the past two decades, with spatial expansion occurring from northwest to southeast. Vegetation coverage exhibits a positive correlation with climate factors. Approximately 60.7% of the area showed a positive correlation between vegetation fractional cover (FVC) and precipitation, with 8.66% of the area demonstrating extremely significant (p < 0.05) and significant (p < 0.01) positive correlation. Human activities, on the whole, have contributed to the enhancement of vegetation cover in the Qinghai-Tibet Plateau. The areas where human activities have positively impacted vegetation cover are primarily situated in north-central Qinghai and north of Ngari, while areas experiencing degradation include certain grassland regions in central-eastern Yushu, Nagqu, and Lhasa.


Assuntos
Monitoramento Ambiental , Atividades Humanas , Humanos , Tibet , Mudança Climática , Ecossistema , China , Temperatura
9.
Arch Biochem Biophys ; 746: 109733, 2023 09 15.
Artigo em Inglês | MEDLINE | ID: mdl-37652148

RESUMO

Pathological scarring is the greatest challenge after injury. Exosome from adipose-derived mesenchymal stem cells has been reported effective to improve hypertrophic scar. This study focused on the possible mechanisms during this process. Exosomes from adipose-derived mesenchymal stem cells were extracted first. Hypertrophic scar tissue and paired normal skin tissue were collected from patients. Mice skin incision model and fibroblasts model were established. TGF-ß1 was used to stimulate fibroblasts to myofibroblasts transdifferentiation. It was found that exosomes injection could decrease collagen sediment after wound healing. During which, the expression of microRNA-181a decreased. Further, we found that expression of microRNA-181a in scar tissue was higher than in normal skin. Then hypertrophic scar-derived fibroblasts were used for in vitro study. It was found that similar to the use of exosomes, microRNA-181a inhibitor decreased the expression of collagen and α-SMA. While microRNA-181a mimics suppressed the effects of exosomes. During fibroblast to myofibroblast trans-differentiation, level of microRNA-181a well as levels of scar-related molecules also decreased with the use of exosomes and vice versa. SIRT1 was confirmed one of the downstream targets of microRNA-181a. Suppression of SIRT1 led to diminished effects of exosomes in hypertrophic scar derived fibroblasts. In mice skin incision model, injection of SIRT1 inhibitor led to increased collagen synthesis. In conclusion, exosomes from Adipose-derived mesenchymal stem cells are promising to antagonize scarring through the regulation of microRNA-181a/SIRT1 axis.


Assuntos
Cicatriz Hipertrófica , Exossomos , Células-Tronco Mesenquimais , MicroRNAs , Animais , Camundongos , Modelos Animais de Doenças , MicroRNAs/genética , Sirtuína 1/genética , Humanos
10.
Macromol Rapid Commun ; 44(18): e2300223, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37249561

RESUMO

Flexible electrolytes with solid self-supporting properties are highly desired in the fields of energy and electronics. However, traditional flexible electrolytes prepared by doping ionic liquids or salt solutions into a polymer matrix pose a risk of liquid component leakage during device operation. In this work, the development of supramolecular ionic network electrolytes using polyoxometalate nanoclusters as supramolecular crosslinkers to solidify bola-type zwitterionic liquids is reported. The resulting self-supporting electrolytes possess semi-solid features and show a high proton conductivity of 8.2 × 10-4 S cm-1 at low humidity (RH = 30%). Additionally, the electrolytes exhibit a typical plateau region in rheological tests, indicating that their dynamic network structures can contribute mechanical behavior similar to the entangled networks in covalent polymer materials. This work introduces a new paradigm for designing flexible solid electrolytes and expands the concept of reticular chemistry to noncrystalline systems.


Assuntos
Eletrólitos , Prótons , Íons , Polímeros
11.
Phytochemistry ; 211: 113690, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37150432

RESUMO

Nigrograna sp. LY66, an endophytic fungus associated with the herbal medicinal plant Clematis shensiensis, produced four undescribed steroids, nigergostanes A-D (1-4), including an unusual ketal-containing nigergostane (1), and four undescribed sesquiterpenoids decorated with cyclohexanone motifs, nigbisabolanes A-D (7-10), along with three known compounds, 23R-hydroxy-(20Z,24R)-ergosta-4,6,8(14),20(22)-tetraen-3-one (5), ergosta-5,7,22-trien-3ß-ol (6), and curculonone A (11). The structures and absolute configurations of these undescribed compounds were confirmed using spectroscopic data (NMR and HRESIMS), modified Mosher's method, and ECD experiments. Additionally, compounds 5 and 8 displayed significant inhibition of nitric oxide generation in lipopolysaccharide-induced BV-2 microglial cells with IC50 values of 2.8 and 2.7 µM, respectively, and is thus more potent than that of the positive control, quercetin (IC50 = 8.77 µM). A molecular docking study revealed that 23-OH of 5 binds to the Y347 residue of inducible nitric oxide synthase (iNOS), whereas the 2-OH and 9,10-diol moieties of 8 bind to R381 and W463 and haeme residues of iNOS, respectively, which has rarely been reported in previous studies. These findings provide a set of undescribed lead compounds that can be developed into anti-neuroinflammatory agents.


Assuntos
Ascomicetos , Clematis , Fitosteróis , Sesquiterpenos , Esteróis , Clematis/metabolismo , Simulação de Acoplamento Molecular , Ascomicetos/metabolismo , Sesquiterpenos/farmacologia , Sesquiterpenos/química , Espectroscopia de Ressonância Magnética , Estrutura Molecular , Óxido Nítrico
12.
Nano Lett ; 23(9): 3887-3896, 2023 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-37094227

RESUMO

Nafion, as the mostly used proton exchange membrane material in vanadium redox flow batteries (VRFBs), encounters serious vanadium permeation problems due to the large size difference between its anionic nanophase (3-5 nm) and cationic vanadium ions (∼0.6 nm). Bulk hybridization usually suppresses the vanadium permeation at the expense of proton conductivity since conventional additives tend to randomly agglomerate and damage the nanophase continuity from unsuitable sizes and intrinsic incompatibility. Here, we report the ionic-nanophase hybridization strategy of Nafion membranes by using fluorinated block copolymers (FBCs) and polyoxometalates (POMs) as supramolecular patching additives. The cooperative noncovalent interactions among Nafion, interfacial-active FBCs, and POMs can construct a 1 nm-shrunk ionic nanophase with abundant proton transport sites, preserved continuity, and efficient vanadium screeners, which leads to a comprehensive enhancement in proton conductivity, selectivity, and VRFB performance. These results demonstrate the intriguing potential of the supramolecular patching strategy in precisely tuning nanostructured electrolyte membranes for improved performance.

13.
ACS Nano ; 16(11): 19240-19252, 2022 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-36315623

RESUMO

Advanced proton exchange membranes (PEMs) are highly desirable in emerging sustainable energy technology. However, the further improvement of commercial perfluorosulfonic acid PEMs represented by Nafion is hindered by the lack of precise modification strategy due to their chemical inertness and low compatibility. Here, we report the robust assembly of polyethylene glycol grafted polyoxometalate amphiphile (GSiW11) into the ionic nanophases of Nafion, which largely enhances the comprehensive performance of Nafion. GSiW11 can coassemble with Nafion through multiple supramolecular interactions and realize a stable immobilization. The incorporation of GSiW11 can increase the whole proton content in the system and induce the hydrated ionic nanophase to form a wide channel for proton transport; meanwhile, GSiW11 can reinforce the Nafion ionic nanophase by noncovalent cross-linking. Based on these synergistic effects, the hybrid PEMs show multiple enhancements in proton conductivity, tensile strength, and fuel cell power density, which are all superior to the pristine Nafion. This work demonstrates the intriguing advantage of molecular nanoclusters as supramolecular enhancers to develop high-performance electrolyte materials.

14.
ACS Omega ; 7(31): 27206-27215, 2022 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-35967013

RESUMO

Lab experiments, field pilots, and numerical modeling focusing on fluid flow aspects have indicated that multi-branch wells are technically effective and promising. Several researchers have conducted some experiments for a fishbone well strategy with mixed results. Our objective in this work is to study the impact of the different fishbone well patterns, such as branch angle, on the distribution of remaining oil after water flooding. In this paper, the interference effect between branches on oil recovery is studied in three steps. First, the interferences between fishbone wells with different branch angles were measured by hydro-electric simulation experiments. Second, two-dimensional visualization water flooding experiments were carried out to clarify the remaining oil distribution at different branch angles. Third, the distribution of oil and water in fishbone wells was verified by establishing a numerical model. The modeling results agree well with the experimental phenomena. At the same time, the variation trend of water and oil production in each branch is analyzed by numerical simulation results. The results indicate that the production is strongly dependent on the branch angles, and the highest recovery was 60.2% at a 45° branch angle.

15.
J Environ Manage ; 321: 115823, 2022 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-35969969

RESUMO

As the total water resources consumption control and carbon mitigation continuous improvement, the weak water-carbon incorporate management is increasingly exposed. In this study, a water-carbon nexus assessment framework is proposed to analyze the nexus relationship between water consumption and carbon emission, and distinguishes the coupled water-carbon transmission intensity and the transfer paths under regional and industrial scales. According to the practical input-output table, water consumption, and carbon emission information, the framework is applied to Beijing-Tianjin-Hebei urban agglomeration (BTHUA), a population, resource, and trade intensive area of China. Inter-regional/intra-regional water consumption and carbon emission transfer fluxes between sectors, the pairwise ecological relationship, and the water-carbon nexus were analyzed. Results indicated that the water-carbon transfer indexes from Hebei to Beijing and Tianjin were 161.85 kg/m3 and 113.88 kg/m3 in the study period, along with the most water consumption and carbon emission, and the worst water-carbon nexus. From the industrial perspective, electricity and gas supplying industry provided 7.8% and 29.1% of the total carbon transfer in Tianjin and Hebei, as the most key node sectors on the water-carbon nexus in the BTHUA. The research provides valuably supporting the adjustment of the existing urban agglomeration water-carbon nexus management schemes.


Assuntos
Carbono , Água , Pequim , China , Cidades , Recursos Hídricos
16.
Nat Nanotechnol ; 17(8): 829-833, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35589820

RESUMO

Photonic quantum technology provides a viable route to quantum communication1,2, quantum simulation3 and quantum information processing4. Recent progress has seen the realization of boson sampling using 20 single photons3 and quantum key distribution over hundreds of kilometres2. Scaling the complexity requires architectures containing multiple photon sources, photon counters and a large number of indistinguishable single photons. Semiconductor quantum dots are bright and fast sources of coherent single photons5-9. For applications, a roadblock is the poor quantum coherence on interfering single photons created by independent quantum dots10,11. Here we demonstrate two-photon interference with near-unity visibility (93.0 ± 0.8)% using photons from two completely separate GaAs quantum dots. The experiment retains all the emission into the zero phonon line-only the weak phonon sideband is rejected; temporal post-selection is not employed. By exploiting quantum interference, we demonstrate a photonic controlled-not circuit and an entanglement with fidelity of (85.0 ± 1.0)% between photons of different origins. The two-photon interference visibility is high enough that the entanglement fidelity is well above the classical threshold. The high mutual coherence of the photons stems from high-quality materials, diode structure and relatively large quantum dot size. Our results establish a platform-GaAs quantum dots-for creating coherent single photons in a scalable way.

17.
Nat Nanotechnol ; 17(5): 436-437, 2022 05.
Artigo em Inglês | MEDLINE | ID: mdl-35474527

Assuntos
Lasers , Fótons , Luz
18.
Sensors (Basel) ; 22(8)2022 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-35458857

RESUMO

Currently, hidden Markov-based multi-step attack detection models are mainly trained using the unsupervised Baum-Welch algorithm. The Baum-Welch algorithm is sensitive to the initial values of model parameters. However, its training uses random or average parameter initialization methods, which frequently results in the model training into a local optimum, thus, making the model unable to fit the alert logs well and thereby reducing the detection effectiveness of the model. To solve this issue, we propose a pre-training method for multi-step attack detection models based on the high semantic similarity of alerts in the same attack phase. The method first clusters the alerts based on their semantic information and pre-classifies the attack phase to which each alert belongs. Then, the distance of the alert vector to each attack stage is converted into the probability of generating alerts in each attack stage, replacing the initial value of Baum-Welch. The effectiveness of the proposed method is evaluated using the DARPA 2000 dataset, DEFCON21 CTF dataset, and ISCXIDS 2012 dataset. The experimental results show that the hidden Markov multi-step attack detection method based on pre-training of the proposed model parameters had higher detection accuracy than the Baum-Welch-based, K-means-based, and transfer learning differential evolution-based hidden Markov multi-step attack detection methods.


Assuntos
Algoritmos , Cadeias de Markov , Probabilidade
19.
J Am Chem Soc ; 143(50): 21433-21442, 2021 Dec 22.
Artigo em Inglês | MEDLINE | ID: mdl-34886669

RESUMO

Modern electrochemical and electronic devices require advanced electrolytes. Liquid crystals have emerged as promising electrolyte candidates due to their good fluidity and long-range order. However, the mesophase of liquid crystals is variable upon heating, which limits their applications as high-temperature electrolytes, e.g., implementing anhydrous proton conduction above 100 °C. Here, we report a highly stable thermotropic liquid-crystalline electrolyte based on the electrostatic self-assembly of polyoxometalate (POM) clusters and zwitterionic polymer ligands. These electrolytes can form a well-ordered mesophase with sub-10 nm POM-based columnar domains, attributed to the dynamic rearrangement of polymer ligands on POM surfaces. Notably, POMs can serve as both electrostatic cross-linkers and high proton conductors, which enable the columnar domains to be high-temperature-stable channels for anhydrous proton conduction. These nanochannels can maintain constant columnar structures in a wide temperature range from 90 to 160 °C. This work demonstrates the unique role of POMs in developing high-performance liquid-crystalline electrolytes, which can provide a new route to design advanced ion transport systems for energy and electronic applications.

20.
Nat Commun ; 12(1): 6575, 2021 Nov 12.
Artigo em Inglês | MEDLINE | ID: mdl-34772948

RESUMO

In a radiative Auger process, optical decay leaves other carriers in excited states, resulting in weak red-shifted satellite peaks in the emission spectrum. The appearance of radiative Auger in the emission directly leads to the question if the process can be inverted: simultaneous photon absorption and electronic demotion. However, excitation of the radiative Auger transition has not been shown, neither on atoms nor on solid-state quantum emitters. Here, we demonstrate the optical driving of the radiative Auger transition, linking few-body Coulomb interactions and quantum optics. We perform our experiments on a trion in a semiconductor quantum dot, where the radiative Auger and the fundamental transition form a Λ-system. On driving both transitions simultaneously, we observe a reduction of the fluorescence signal by up to 70%. Our results suggest the possibility of turning resonance fluorescence on and off using radiative Auger as well as THz spectroscopy with optics close to the visible regime.

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