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1.
Front Plant Sci ; 12: 743781, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34691121

RESUMO

Metabolites are major contributors to the quality of tea that are regulated by various abiotic stresses. Light intensity and phosphorus (P) supply affect the metabolism of tea plants. However, how these two factors interact and mediate the metabolite levels in tea plants are not fully understood. The present study investigated the consequences of different light intensity and P regimes on the metabolism of carbohydrates, amino acids, and flavonoids in the Fengqing tea cultivar. The leaves and young shoots were subjected to untargeted metabolomics analysis by two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC×GC-TOF/MS), ultra-performance liquid chromatography-quadrupole-TOF/MS (UPLC-Q-TOF/MS), and targeted analysis by high-performance liquid chromatography (HPLC) along with quantification of gene expression by quantitative real time-PCR (qRT-PCR). The results from young shoots showed that amino acids, pentose phosphate, and flavonol glycosides pathways were enhanced in response to decreasing light intensities and P deficiency. The expression of the genes hexokinase 1, ribose 5-phosphate isomerase A (RPIA), glutamate synthetase 1 (GS1), prolyl 4-hydroxylase (P4H), and arginase was induced by P limitation, thereafter affecting carbohydrates and amino acids metabolism, where shading modulated the responses of transcripts and corresponding metabolites caused by P deficiency. P deprivation repressed the expression of Pi transport, stress, sensing, and signaling (SPX2) and induced bidirectional sugar transporter (SWEET3) and amino acid permeases (AAP) which ultimately caused an increase in the amino acids: glutamate (Glu), proline (Pro), and arginine (Arg) under shading but decreased catechins [epicatechingallate (ECG) and Gallic acid, GA] content in young shoots.

2.
Nat Commun ; 10(1): 3064, 2019 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-31296880

RESUMO

The unique properties of ferroelectric materials enable a plethora of applications, which are hindered by the phenomenon known as ferroelectric fatigue that leads to the degradation of ferroelectric properties with polarization cycling. Multiple microscopic models explaining fatigue have been suggested; however, the chemical origins remain poorly understood. Here, we utilize multimodal chemical imaging that combines atomic force microscopy with time-of-flight secondary mass spectrometry to explore the chemical phenomena associated with fatigue in PbZr0.2Ti0.8O3 (PZT) thin films. Investigations reveal that the degradation of ferroelectric properties is correlated with a local chemical change and migration of electrode ions into the PZT structure. Density functional theory simulations support the experimental results and demonstrate stable doping of the thin surface PZT layer with copper ions, leading to a decrease in the spontaneous polarization. Overall, the performed research allows for the observation and understanding of the chemical phenomena associated with polarization cycling and their effects on ferroelectric functionality.

4.
Nano Lett ; 19(2): 1033-1038, 2019 02 13.
Artigo em Inglês | MEDLINE | ID: mdl-30673240

RESUMO

In classical morphotropic piezoelectric materials, rhombohedral and tetragonal phase variants can energetically compete to form a mixed phase regime with improved functional properties. While the discovery of morphotropic-like phases in multiferroic BiFeO3 films has broadened this definition, accessing these phase spaces is still typically accomplished through isovalent substitution or heteroepitaxial strain which do not allow for continuous modification of phase composition postsynthesis. Here, we show that it is possible to use low-energy helium implantation to tailor morphotropic phases of epitaxial BiFeO3 films postsynthesis in a continuous and iterative manner. Applying this strain doping approach to morphotropic films creates a new phase space based on internal and external lattice stress that can be seen as an analogue to temperature-composition phase diagrams of classical morphotropic ferroelectric systems.

5.
Int J Mol Sci ; 19(11)2018 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-30469347

RESUMO

The qualities of tea (Camellia sinensis) are not clearly understood in terms of integrated leading molecular regulatory network mechanisms behind inorganic phosphate (Pi) limitation. Thus, the present work aims to elucidate transcription factor-dependent responses of quality-related metabolites and the expression of genes to phosphate (P) starvation. The tea plant organs were subjected to metabolomics analysis by GC×GC-TOF/MS and UPLC-Q-TOF/MS along with transcription factors and 13 metabolic genes by qRT-PCR. We found P starvation upregulated SPX2 and the change response of Pi is highly dependent on young shoots. This led to increased change in abundance of carbohydrates (fructose and glucose), amino acids in leaves (threonine and methionine), and root (phenylalanine, alanine, tryptophan, and tyrosine). Flavonoids and their glycosides accumulated in leaves and root exposed to P limitation was consistent with the upregulated expression of anthocyanidin reductase (EC 1.3.1.77), leucoanthocyanidin dioxygenase (EC 1.4.11.19) and glycosyltransferases (UGT78D1, UGT78D2 and UGT57L12). Despite the similar kinetics and high correlation response of Pi and SPX2 in young shoots, predominating theanine and other amino acids (serine, threonine, glutamate, valine, methionine, phenylalanine) and catechin (EGC, EGCG and CG) content displayed opposite changes in response to Pi limitation between Fengqing and Longjing-43 tea cultivars.


Assuntos
Aminoácidos/metabolismo , Camellia sinensis/metabolismo , Flavonoides/metabolismo , Fosfatos/deficiência , Camellia sinensis/genética , Glicosiltransferases/genética , Glicosiltransferases/metabolismo , Oxigenases/genética , Oxigenases/metabolismo , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo , Estresse Fisiológico
6.
ACS Omega ; 2(6): 2827-2834, 2017 Jun 30.
Artigo em Inglês | MEDLINE | ID: mdl-31457620

RESUMO

Atomic structures and electronic properties of MoS2/HfO2 defective interfaces are investigated extensively for future field-effect transistor device applications. To mimic the atomic layer deposition growth under ambient conditions, the impact of interfacial oxygen concentration on the MoS2/HfO2 interface electronic structure is examined. Then, the effect on band offsets (BOs) and the thermodynamic stability of those interfaces is investigated and compared with available relevant experimental data. Our results show that the BOs can be modified up to 2 eV by tuning the oxygen content through, for example, the relative partial pressure. Interfaces with hydrogen impurities as well as various structural disorders were also considered, leading to different behaviors, such as n-type doping, or introducing defect states close to the Fermi level because of the formation of hydroxyl groups. Then, our results indicate that for a well-prepared interface the electronic device performance should be better than that of other interfaces, such as III-V/high-κ, because of the absence of interface defect states. However, any unpassivated defects, if present during oxide growth, strongly affect the subsequent electronic properties of the interface. The unique electronic properties of monolayer-to-few-layered transition-metal dichalcogenides and dielectric interfaces are described in detail for the first time, showing the promising interfacial characteristics for future transistor technology.

7.
Sci Rep ; 6: 29184, 2016 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-27378032

RESUMO

Semiconductors with a moderate bandgap have enabled modern electronic device technology, and the current scaling trends down to nanometer scale have introduced two-dimensional (2D) semiconductors. The bandgap of a semiconductor has been an intrinsic property independent of the environments and determined fundamental semiconductor device characteristics. In contrast to bulk semiconductors, we demonstrate that an atomically thin two-dimensional semiconductor has a bandgap with strong dependence on dielectric environments. Specifically, monolayer MoS2 bandgap is shown to change from 2.8 eV to 1.9 eV by dielectric environment. Utilizing the bandgap modulation property, a tunable bandgap transistor, which can be in general made of a two-dimensional semiconductor, is proposed.

8.
ACS Nano ; 10(8): 7370-5, 2016 08 23.
Artigo em Inglês | MEDLINE | ID: mdl-27415610

RESUMO

Metal-insulator transitions in low-dimensional materials under ambient conditions are rare and worth pursuing due to their intriguing physics and rich device applications. Monolayer MoTe2 and WTe2 are distinguished from other TMDs by the existence of an exceptional semimetallic distorted octahedral structure (T') with a quite small energy difference from the semiconducting H phase. In the process of transition metal alloying, an equal stability point of the H and the T' phase is observed in the formation energy diagram of monolayer WxMo1-xTe2. This thermodynamically driven phase transition enables a controlled synthesis of the desired phase (H or T') of monolayer WxMo1-xTe2 using a growth method such as chemical vapor deposition (CVD) and molecular beam epitaxy (MBE). Furthermore, charge mediation, as a more feasible method, is found to make the T' phase more stable than the H phase and induce a phase transition from the H phase (semiconducting) to the T' phase (semimetallic) in monolayer WxMo1-xTe2 alloy. This suggests that a dynamic metal-insulator phase transition can be induced, which can be exploited for rich phase transition applications in two-dimensional nanoelectronics.

9.
Science ; 350(6264): 1065-8, 2015 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-26612948

RESUMO

Two-dimensional (2D) transition metal dichalcogenides have emerged as a promising material system for optoelectronic applications, but their primary figure of merit, the room-temperature photoluminescence quantum yield (QY), is extremely low. The prototypical 2D material molybdenum disulfide (MoS2) is reported to have a maximum QY of 0.6%, which indicates a considerable defect density. Here we report on an air-stable, solution-based chemical treatment by an organic superacid, which uniformly enhances the photoluminescence and minority carrier lifetime of MoS2 monolayers by more than two orders of magnitude. The treatment eliminates defect-mediated nonradiative recombination, thus resulting in a final QY of more than 95%, with a longest-observed lifetime of 10.8 ± 0.6 nanoseconds. Our ability to obtain optoelectronic monolayers with near-perfect properties opens the door for the development of highly efficient light-emitting diodes, lasers, and solar cells based on 2D materials.

10.
ACS Nano ; 9(2): 1543-51, 2015 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-25494557

RESUMO

The experimental study of interlayer sliding at the nanoscale in layered solids has been limited thus far by the incapability of mechanical and imaging probes to simultaneously access sliding interfaces and overcome through mechanical stimulus the van der Waals and Coulombic interactions holding the layers in place. For this purpose, straightforward methods were developed to achieve interlayer sliding in molybdenum disulfide (MoS2) while under observation within a transmission electron microscope. A method to manipulate, tear, and slide free-standing atomic layers of MoS2 is demonstrated by electrostatically coupling it to an oxidized tungsten probe attached to a micromanipulator at a bias above ±7 V. A first-principles model of a MoS2 bilayer polarized by a normal electric field of 5 V/nm, emanating from the tip, demonstrates the appearance of a periodic negative sliding potential energy barrier when the layers slide into the out-of-registry stacking configuration, hinting at electrostatic gating as a means of modifying the interlayer tribology to facilitate shear exfoliation. A method to shear focused ion beam prepared MoS2 cross section samples using a nanoindenter force sensor is also demonstrated, allowing both the observation and force measurement of its interlayer dynamics during shear-induced sliding. From this experiment, the zero normal load shear strength of MoS2 can be directly obtained: 25.3 ± 0.6 MPa. These capabilities enable the site-specific mechanical testing of dry lubricant-based nanoelectromechanical devices and can lead to a better understanding of the atomic mechanisms from which the interlayer tribology of layered materials originates.

11.
Phys Chem Chem Phys ; 16(23): 11218-27, 2014 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-24776820

RESUMO

In this work, we present a density-functional theory (DFT) investigation of the phase stability, electrochemical stability and phase transformation mechanisms of the layered and over-lithiated Mn oxides. This study includes the thermodynamic stability of Li and oxygen vacancies, to examine the electrochemical activation mechanisms of these cathode materials. The DFT calculations provide phase diagrams of the Li-Mn-O system in both physical and chemical potential spaces, including the crystals containing vacancies as independent phases. The results show the ranges of electrochemical activity for both layered LiMnO2 and over-lithiated Li2MnO3. By using a thermodynamic model analysis, we found that the required temperature for oxygen evolution and Li vacancy formation is too high to be compatible with any practical synthesis temperature. Using solid-state transition calculations, we have identified the key steps in the phase transition mechanism of the layered LiMnO2 into the spinel phase. The calculated effects of pH on the Li-Mn-O phase stability elucidated the mechanism of Mn(2+) formation from the spinel phase under acidic conditions.

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