首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 437 毫秒
1.
  相似文献   

2.
The strong spatial confinement of a nanocavity plasmonic field has made it possible to visualize the inner structure of a single molecule and even to distinguish its vibrational modes in real space. With such ever-improved spatial resolution, it is anticipated that full vibrational imaging of a molecule could be achieved to reveal molecular structural details. Here we demonstrate full Raman images of individual vibrational modes at the ångström level for a single Mg-porphine molecule, revealing distinct characteristics of each vibrational mode in real space. Furthermore, by exploiting the underlying interference effect and Raman fingerprint database, we propose a new methodology for structural determination, which we have called ‘scanning Raman picoscopy’, to show how such ultrahigh-resolution spectromicroscopic vibrational images can be used to visually assemble the chemical structure of a single molecule through a simple Lego-like building process.  相似文献   

3.
Waveguides and resonators are core components in the large-scale integration of electronics, photonics and phononics, both in existing and future scenarios. In certain situations, there is critical coupling of the two components; i.e. no energy passes through the waveguide after the incoming wave couples into the resonator. The transmission spectral characteristics resulting from this phenomenon are highly advantageous for signal filtering, switching, multiplexing and sensing. In the present study, adopting an elastic-wave platform, we introduce topological insulator (TI), a remarkable achievement in condensed matter physics over the past decade, into a classical waveguide-ring-resonator configuration. Along with basic similarities with classical systems, a TI system has important differences and advantages, mostly owing to the spin-momentum locked transmission states at the TI boundaries. As an example, a two-port TI waveguide resonator can fundamentally eliminate upstream reflections while completely retaining useful transmission spectral characteristics, and maximize the energy in the resonator, with possible applications being novel signal processing, gyro/sensing, lasering, energy harvesting and intense wave–matter interactions, using phonons, photons or even electrons. The present work further enhances confidence in using topological protection for practical device performance and functionalities, especially considering the crucial advantage of introducing (pseudo)spins to existing conventional configurations. More in-depth research on advancing phononics/photonics, especially on-chip, is foreseen.  相似文献   

4.
Nonfullerene acceptors are being investigated for use in polymer solar cells (PSCs), with their advantages of extending the absorption range, reducing the energy loss and therefore enhancing the power conversion efficiency (PCE). However, to further boost the PCE, mobilities of these nonfullerene acceptors should be improved. For nonfullerene acceptors, the π–π stacking distance between cofacially stacked molecules significantly affects their mobility. Here, we demonstrate a strategy to increase the mobility of heteroheptacene-based nonfullerene acceptors by reducing their π–π stacking distances via control over the bulkiness of lateral side chains. Incorporation of 2-butyloctyl substituents into the nonfullerene acceptor (M36) leads to an increased mobility with a reduced π–π stacking distance of 3.45 Å. Consequently, M36 affords an enhanced PCE of 16%, which is the highest among all acceptor-donor-acceptor-type nonfullerene acceptors to date. This strategy of control over the bulkiness of side chains on nonfullerene acceptors should aid the development of more efficient PSCs.  相似文献   

5.
综述了近几年来关于三原子分子离子(CS+2, SO+2, CO+2)的光激发和光解离动力学研究结果.实验是在射流气束条件下进行的.首先利用一束电离激光使中性三原子分子通过共振增强多光子电离制备出振动态选择的三原子分子离子,再用一束或两束解离激光激发获得母体分子离子的光解离谱(母体离子的凹陷谱和碎片离子的增强谱).由此研究了三原子分子离子(CS+2, SO+2, CO+2)电子态的光激发和光解离动力学.  相似文献   

6.
The theory of vibrational control is developed. The necessary and sufficient conditions for vibrational stabilizability of linear dynamic systems are found. Basic relations of the vibrational control method and the optimal shape of vibrations are determined. Unlike conventional methods, based on feedback or feedforward principles, the method of the paper does not require measurement of the deviations or disturbances.  相似文献   

7.
Despite extensive research and several stunning breakthroughs in the synthesis of interlocked molecular species, [3]catenanes, Borromean rings and ring-in-ring complexes are exceedingly rare and their targeted synthesis remains a formidable challenge. Herein, a series of Cp*Rh-based homogeneous and heterogeneous interlocked structures have been prepared by coordination-driven self-assembly, not only including metalla[2]catenanes and molecular Borromean rings, but also linear metalla[3]catenanes and ring-in-ring complexes. The interlocked structures are all based on bithiophenyl groups. The bithiophenyl groups effectively enhance the strength of the inter-ring interactions and play a crucial role in the formation of these interlocked structures. By taking advantage of the strong interaction between π-donor (D) and π-acceptor (A) groups, the electron-deficient methylviologen cation was introduced into a cationic metallarectangle based on bithiophenyl groups. Taking inspiration from these results, a cationic metallarectangle based on A units was threaded into a metallarectangle based on D units, leading to a heterogeneous D–A ring-in-ring structure.  相似文献   

8.
N-heterocyclic phosphines (NHPs) have recently emerged as a new group of promising catalysts for metal-free reductions, owing to their unique hydridic reactivity. The excellent hydricity of NHPs, which rivals or even exceeds those of many metal-based hydrides, is the result of hyperconjugative interactions between the lone-pair electrons on N atoms and the adjacent σ*(P–H) orbital. Compared with the conventional protic reactivity of phosphines, this umpolung P–H reactivity leads to hydridic selectivity in NHP-mediated reductions. This reactivity has therefore found many applications in the catalytic reduction of polar unsaturated bonds and in the hydroboration of pyridines. This review summarizes recent progress in studies of the reactivity and synthetic applications of these phosphorus-based hydrides, with the aim of providing practical information to enable exploitation of their synthetically useful chemistry.  相似文献   

9.
Links in most real networks often change over time. Such temporality of links encodes the ordering and causality of interactions between nodes and has a profound effect on network dynamics and function. Empirical evidence has shown that the temporal nature of links in many real-world networks is not random. Nonetheless, it is challenging to predict temporal link patterns while considering the entanglement between topological and temporal link patterns. Here, we propose an entropy-rate-based framework, based on combined topological–temporal regularities, for quantifying the predictability of any temporal network. We apply our framework on various model networks, demonstrating that it indeed captures the intrinsic topological–temporal regularities whereas previous methods considered only temporal aspects. We also apply our framework on 18 real networks of different types and determine their predictability. Interestingly, we find that, for most real temporal networks, despite the greater complexity of predictability brought by the increase in dimension, the combined topological–temporal predictability is higher than the temporal predictability. Our results demonstrate the necessity for incorporating both temporal and topological aspects of networks in order to improve predictions of dynamical processes.  相似文献   

10.
Designing new cathodes with high capacity and moderate potential is the key to breaking the energy density ceiling imposed by current intercalation chemistry on rechargeable batteries. The carbonaceous materials provide high capacities but their low potentials limit their application to anodes. Here, we show that Fermi level tuning by p-type doping can be an effective way of dramatically raising electrode potential. We demonstrate that Li(Na)BCF2/Li(Na)B2C2F2 exhibit such change in Fermi level, enabling them to accommodate Li+(Na+) with capacities of 290–400 (250–320) mAh g−1 at potentials of 3.4–3.7 (2.7–2.9) V, delivering ultrahigh energy densities of 1000–1500 Wh kg−1. This work presents a new strategy in tuning electrode potential through electronic band structure engineering.  相似文献   

11.
Knowledge of intrinsic wettability at solid/liquid interfaces at the molecular level perspective is significant in understanding crucial progress in some fields, such as electrochemistry, molecular biology and earth science. It is generally believed that surface wettability is determined by the surface chemical component and surface topography. However, when taking molecular structures and interactions into consideration, many intriguing phenomena would enrich or even redress our understanding of surface wettability. From the perspective of interfacial water molecule structures, here, we discovered that the intrinsic wettability of crystal metal oxide is not only dependent on the chemical components but also critically dependent on the crystal faces. For example, the crystal face of α-Al2O3 is intrinsically hydrophobic with a water contact angle near 90°, while another three crystal faces are intrinsically hydrophilic with water contact angles <65°. Based on surface energy analysis, it is found that the total surface energy, polar component and Lewis base portion of the hydrophobic crystal face are all smaller than the other three hydrophilic crystal faces indicating that they have different surface states. DFT simulation further revealed that the adsorbed interfacial water molecules on each crystal face hold various orientations. Herein, the third crucial factor for surface wettability from the perspective of the molecular level is presented, that is the orientations of adsorbed interfacial water molecules apart from the macro-level chemical component and surface topography. This study may serve as a source of inspiration for improving wetting theoretical models and designing controllable wettability at the molecular/atomic level.  相似文献   

12.
The classical problem of broadband matching was first studied by Bode (1) and developed later by Fano (2); however, Fano's solution, although very elegant, has a practical limitation. The key idea is to replace the load Z2(S) by its Darlington equivalent ending in 1 ohm, but the optimum design is, in general, not very simple. Youla (3) proposed an alternative method where it is relatively easy to find the optimum network even for the more complex impedance load. The paper shows that maximization of the gainbandwidth product, in the presence of load or source variations, depends on the choice of the reflection coefficient zeros, either in the left half-plane or in the right half-plane.  相似文献   

13.
The westward expansion of human millet consumption from north China has important implications for understanding early interactions between the East and West. However, few studies have focused on the Xinjiang Uyghur Autonomous Region, the vast geographical area directly linking the ancient cultures of the Eurasian Steppe and the Gansu Corridor of China. In this study, we present the largest isotopic investigation of Bronze Age China (n = 110) on material from the key site of Tianshanbeilu, in eastern Xinjiang. The large range of δ13C values (–17.6‰ to –7.2‰; –15.5 ± 1.2‰) provides direct evidence of unique dietary diversity and consumption of significant C4 resources (millets). The high δ15N results (10.3‰ to 16.7‰; 14.7 ± 0.8‰) likely reflect sheep/goat and wild game consumption and the arid climate of the Taklamakan Desert. Radiocarbon dates from four individuals indicate Tianshanbeilu was in use between 1940 and 1215 cal bc. The Tianshanbeilu results are then analysed with respect to 52 Bronze Age sites from across Eurasia, to investigate the spread and chronology of significant human millet consumption and human migration. This isotopic survey finds novel evidence that the second millennium bc was a dynamic period, with significant dietary interconnectivity occurring between north China, Central Asia and Siberia. Further, we argue that this ‘Isotopic Millet Road’ extended all the way to the Mediterranean and Central Europe, and conclude that these C4 dietary signatures of millet consumption reflect early links (migration and/or resource transfer) between the Bronze Age inhabitants of modern-day China and Europe.  相似文献   

14.
Since solar energy is the ultimate energy resource and a significant amount of global energy utilization goes through heat, there have been persistent efforts for centuries to develop devices and systems for solar–thermal conversion. Most recently, interfacial solar vapor generation, as an emerging concept of solar–thermal conversion, has gained significant attention for its great potentials in various fields such as desalination, sterilization, catalysis, etc. With the advances of rationally designed materials and structures and photon and thermal management at the nanoscale, interfacial solar vapor generation has demonstrated both thermodynamic and kinetical advantages over conventional strategies. In this review, we aim to illustrate the definition, mechanism and figures of merit of interfacial solar vapor generation, and to summarize the development progress of relevant materials and applications, as well as to provide a prospective view of the future.  相似文献   

15.
Contact interface properties are important in determining the performances of devices that are based on atomically thin two-dimensional (2D) materials, especially for those with short channels. Understanding the contact interface is therefore important to design better devices. Herein, we use scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations to reveal the electronic structures within the metallic (1T′)-semiconducting (2H) MoTe2 coplanar phase boundary across a wide spectral range and correlate its properties to atomic structures. We find that the 2H-MoTe2 excitonic peaks cross the phase boundary into the 1T′ phase within a range of approximately 150 nm. The 1T′-MoTe2 crystal field can penetrate the boundary and extend into the 2H phase by approximately two unit-cells. The plasmonic oscillations exhibit strong angle dependence, that is a red-shift of π+σ (approximately 0.3–1.2 eV) occurs within 4 nm at 1T′/2H-MoTe2 boundaries with large tilt angles, but there is no shift at zero-tilted boundaries. These atomic-scale measurements reveal the structure–property relationships of the 1T′/2H-MoTe2 boundary, providing useful information for phase boundary engineering and device development based on 2D materials.  相似文献   

16.
Lithium–sulfur batteries have great potential for high-performance energy-storage devices, yet the severe diffusion of soluble polysulfide to electrolyte greatly limits their practical applications. To address the above issues, herein we design and synthesize a novel polymer binder with single lithium-ion channels allowing fast lithium-ion transport while blocking the shuttle of unnecessary polysulfide anions. In situ UV–vis spectroscopy measurements reveal that the prepared polymer binder has effective immobilization to polysulfide intermediates. As expected, the resultant sulfur cathode achieves an excellent specific capacity of 1310 mAh g−1 at 0.2 C, high Coulombic efficiency of 99.5% at 0.5 C after 100 cycles and stable cycling performance for 300 cycles at 1 C (1 C = 1675 mA g−1). This study reports a new avenue to assemble a polymer binder with a single lithium-ion channel for solving the serious problem of energy attenuation of lithium–sulfur batteries.  相似文献   

17.
Multiple myeloma (MM) is diagnosed and monitored by correlating panel of test results including serum Protein electrophoresis (SPE), Immunofixation electrophoresis (IFE), serum Free Light chain (sFLC) measurements. This audit is aimed to evaluate the prevalence of non-correlation and discrepancies amongst the three investigations (SPE/IFE/sFLC) for assessment of MM. 106 MM patients were reviewed over 16 months in a tertiary cancer care center by the availability of 3 serum test results (SPE/IFE/sFLC). Patients were divided into 2 groups: group1, newly diagnosed MM patients who were yet to receive myeloma specific treatment (n = 48); and group2, already diagnosed MM patients on treatment and followup (n = 58). Treatment modalities included stem cell transplantation and standard chemotherapy regimens. Non-correlation between the three test results (IFE/SPE/sFLC) was observed (21% in group1 and 45% in group2). Three types of discrepancies were detected as follows: (a) IFE showing less number of restriction bands as compared to SPE (8.6% patients in group2); (b) SPE/IFE negative with an abnormal sFLC ratio (12.5% patients in group1 and 13.7% in group2); (c) SPE/IFE positive but normal sFLC ratio (8% in group1 and 22% in group2). To conclude, IFE may sometimes provide information that does not always correlate with either of the SPE or sFLC results due to different sensitivities, antigen–antibody interactions, or treatment. Hence, SPE plus sFLC may be more useful particularly for patients on follow-up while IFE plus sFLC may help screen the new patients. The judicious selection of the biochemical assays can effectively reduce the treatment cost in a developing country like India.  相似文献   

18.
A new mechanism of new particle formation (NPF) is investigated using comprehensive measurements of aerosol physicochemical quantities and meteorological variables made in three continents, including Beijing, China; the Southern Great Plains site in the USA; and SMEAR II Station in Hyytiälä, Finland. Despite the considerably different emissions of chemical species among the sites, a common relationship was found between the characteristics of NPF and the stability intensity. The stability parameter (ζ = Z/L, where Z is the height above ground and L is the Monin–Obukhov length) is found to play an important role; it drops significantly before NPF as the atmosphere becomes more unstable, which may serve as an indicator of nucleation bursts. As the atmosphere becomes unstable, the NPF duration is closely related to the tendency for turbulence development, which influences the evolution of the condensation sink. Presumably, the unstable atmosphere may dilute pre-existing particles, effectively reducing the condensation sink, especially at coarse mode to foster nucleation. This new mechanism is confirmed by model simulations using a molecular dynamic model that mimics the impact of turbulence development on nucleation by inducing and intensifying homogeneous nucleation events.  相似文献   

19.
Inertial microfluidics has brought enormous changes in the conventional cell/particle detection process and now become the main trend of sample pretreatment with outstanding throughput, low cost, and simple control method. However, inertial microfluidics in a straight microchannel is not enough to provide high efficiency and satisfying performance for cell/particle separation. A contraction–expansion microchannel is a widely used and multifunctional channel pattern involving inertial microfluidics, secondary flow, and the vortex in the chamber. The strengthened inertial microfluidics can help us to focus particles with a shorter channel length and less processing time. Both the vortex in the chamber and the secondary flow in the main channel can trap the target particles or separate particles based on their sizes more precisely. The contraction–expansion microchannels are also capable of combining with a curved, spiral, or serpentine channel to further improve the separation performance. Some recent studies have focused on the viscoelastic fluid that utilizes both elastic forces and inertial forces to separate different size particles precisely with a relatively low flow rate for the vulnerable cells. This article comprehensively reviews various contraction–expansion microchannels with Newtonian and viscoelastic fluids for particle focusing, separation, and microfluid mixing and provides particle manipulation performance data analysis for the contraction–expansion microchannel design.  相似文献   

20.
Chang’E-4 landed in the South Pole-Aitken (SPA) basin, providing a unique chance to probe the composition of the lunar interior. Its landing site is located on ejecta strips in Von Kármán crater that possibly originate from the neighboring Finsen crater. A surface rock and the lunar regolith at 10 sites along the rover Yutu-2 track were measured by the onboard Visible and Near-Infrared Imaging Spectrometer in the first three lunar days of mission operations. In situ spectra of the regolith have peak band positions at 1 and 2 μm, similar to the spectral data of Finsen ejecta from the Moon Mineralogy Mapper, which confirms that the regolith''s composition of the landing area is mostly similar to that of Finsen ejecta. The rock spectrum shows similar band peak positions, but stronger absorptions, suggesting relatively fresh exposure. The rock may consist of 38.1 ± 5.4% low-Ca pyroxene, 13.9 ± 5.1% olivine and 48.0 ± 3.1% plagioclase, referred to as olivine-norite. The plagioclase-abundant and olivine-poor modal composition of the rock is inconsistent with the origin of the mantle, but representative of the lunar lower crust. Alternatively, the rock crystallized from the impact-derived melt pool formed by the SPA-impact event via mixing the lunar crust and mantle materials. This scenario is consistent with fast-cooling thermal conditions of a shallow melt pool, indicated by the fine to medium-sized texture (<3 mm) of the rock and the SPA-impact melting model [Icarus 2012; 220: 730–43].  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号