Efficient Green Procedure for the Synthesis of Coumarin Derivatives by a One‐Pot,Three‐Component Reaction under Solvent‐Free Conditions

A simple, efficient, and general method has been developed for the synthesis of coumarin derivatives through a one‐pot reaction of aromatic aldehydes, 2,2‐dimethyl‐1,3‐dioxane‐4,6‐dione and 5,5‐dimethyl‐1,3‐cyclohexanedione, in the presence of TEBA under solvent‐free conditions using grinding methods. The mild reaction conditions, simple protocol, high yields, and cleaner reaction make this protocol practical and economically attractive.     

Biginelli-Like Cyclocondensation Reaction: Efficient Synthesis of 4,6-Diarylpyrimidin-2(1H)-one Under Solvent-Free Conditions

An efficient and facile synthesis of 4,6-diarylpyrimidin-2(1H)-one via a Biginelli-like reaction of aromatic aldehydes, aromatic ketones, and urea in the presence of NaOH under solvent-free conditions using a heating method has been developed. Compared with the classical reaction conditions, this new synthetic method has the advantages of excellent yields, shorter reaction time, and mild reaction conditions.      

Multifractal analysis for Cu/Ti bilayer thin films

Two bilayer thin films with different stacking sequences, Cu/Ti/Si and Ti/Cu/Si, were deposited by DC magnetron sputtering technique. X‐ray diffraction technique was used to measure the crystallization structures, and scanning electron microscopy and atomic force microscopy were used to measured surface morphology. The multifractal spectra f(α)‐α was used to characterize the surface morphology. The result of |q|_max ≤ 53 is obtained by multifractal analysis. The shape of the multifractal spectra f(α) ? α is hook‐like for Cu/Ti/Si and bell jar‐like for Ti/Cu/Si. The spectrum width Δα = α_max ? α_min and Δf(=f(α_min) ? f(α_max)) of the multifractal spectra is able to quantitatively analyze the growth and surface roughness of the Cu/Ti bilayer thin films. The surface of Ti/Cu/Si thin film is more uniform and smoother than the film of Cu/Ti/Si. Copyright © 2013 John Wiley & Sons, Ltd.     

A sensitive immunosorbent bio-barcode assay based on real-time immuno-PCR for detecting 3,4,3',4'-tetrachlorobiphenyl

A functionalized gold-nanoparticle bio-barcode assay, based on real-time immuno-PCR (IPCR), was designed for the determination of 3,4,3',4'-tetrachlorobiphenyl (PCB77). 15 nm gold nanoparticles were synthesized, and modified with thiol-capped DNA and goat anti-rabbit IgG. The nanoparticle probes were used to replace antibody–DNA conjugate in the IPCR, and were fixed on the PCR tube wall via the immune reaction. Real-time PCR was performed to quantify the DNA signal directly. Under optimized conditions, the new method was used to detect PCB77 with a linearity range from 5 pg L^?1 to 10 ng L^?1, and the limit of detection (LOD) was 1.72 pg L^?1. Real samples of Larimichthys polyactis, collected from the East China Sea, were analyzed. Recovery was from 82 % to 112 %, and the coefficient of variation (CV) was acceptable. The results were compared with GC–ECD, revealing that the method would be acceptable for providing rapid, semi-quantitative, and reliable test results for making environmental decisions.

Generation of sub‐terahertz repetition rates from a monolithic self‐mode‐locked laser coupled with an external Fabry‐Perot cavity

A novel scheme to multiply the repetition rate of a monolithic self‐mode‐locked laser for generating sub‐terahertz pulse sources is successfully demonstrated. A coated Yb:KGW crystal is designed to achieve a self‐mode‐locked operation at a repetition rate of 24 GHz with an average output power exceeding 1.0 W at a pump power of 4.8 W. A partially reflective mirror is utilized to combine with the output surface of the gain medium to constitute an external Fabry‐Perot cavity. It is theoretically and experimentally verified that adjusting the external cavity length to satisfy the commensurate condition can lead to the frequency spacing to be various order harmonics of the mode spacing of the monolithic cavity. The maximum pulse repetition rate of the laser output can be up to 216 GHz and the pulse duration is as short as 330 fs. More importantly, the overall characteristics of the first‐order temporal autocorrelation traces obtained by sequentially scanning the external cavity.length display an intriguing phenomenon of temporally fractional revivals, similar to the feature of spatial Talbot revivals.

     

空心NiCo2S4纳米球助催化剂担载ZnIn2S4纳米片用于可见光催化制氢

纳米片与空心球上之间的合理界面调控是开发高效太阳能制氢光催化剂的潜在策略。在各类光催化材料中,金属硫化物由于具有相对较窄的带隙和优越的可见光响应能力而被广泛研究。ZnIn₂S₄是一种层状的三元过渡金属半导体光催化剂,其带隙可控(约2.4 eV)。在众多金属硫化物光催化剂中,ZnIn₂S₄引起了广泛兴趣。然而,单纯的ZnIn₂S₄光催化活性仍然相对较差,主要是因为光生载流子的复合率较高、迁移速率较慢。在半导体光催化剂上负载助催化剂是提升光催化剂性能的一种有效方法,因为它不仅可以加速光生电子和空穴的分离,而且还可以降低质子还原反应的活化能。作为一种三元过渡金属硫化物,NiCo₂S₄表现出较高的导电性、较低的电负性、丰富的氧化还原特性以及优越的电催化活性。这些特性表明,NiCo₂S₄可以作为光催化制氢的助催化剂,以加速电荷分离和转移。此外,NiCo₂S₄和ZnIn₂S₄都属于三元尖晶石的晶体结构,这可能有助于构建具有紧密界面接触的NiCo₂S₄/ZnIn₂S₄复合物,从而提高光催化性能。本文中,将超薄ZnIn₂S₄纳米片原位生长到非贵金属助催化剂NiCo₂S₄空心球上,形成具有强耦合界面和可见光吸收的NiCo₂S₄@ZnIn₂S₄分级空心异质结构光催化剂。最优NiCo₂S₄@ZnIn₂S₄复合样品(NiCo₂S₄含量：ca. 3.1%)的析氢速率高达78 μmol·h^-1,约是纳米片组装ZnIn₂S₄光催化剂析氢速率的9倍、约是1% (w, 质量分数)Pt/ZnIn₂S₄样品析氢速率的3倍。此外,该复合光催化剂在反应中表现出良好的稳定性。荧光和电化学测试结果表明,NiCo₂S₄空心球是一种有效的助催化剂,可促进光生载流子的分离和传输,并降低析氢反应的活化能。最后,提出了NiCo₂S₄@ZnIn₂S₄光催化析氢的可能反应机理。在NiCo₂S₄@ZnIn₂S₄复合光催化剂中,具有高导电性的NiCo₂S₄助催化剂可快速接受ZnIn₂S₄上的光生电子,用以还原质子生成氢气,而电子牺牲剂TEOA捕获光生空穴,进而完成光催化氧化还原循环。该研究有望为基于纳米片为次级结构的分级空心异质结光催化剂的设计合成及其光催化制氢研究提供一定的指导。     

Neutral 1D Perovskite-Type ABX3 Phase Transition Material with a Narrowband Emission and Semiconductor Property

Cyclic organic amines are emerging as excellent building blocks to assemble organic–inorganic hybrid phase transition materials due to their flexible cyclic structure. Here, we have assembled a 1D organic-inorganic hybrid dielectric material C₅H₆NOPbBr₃ ( 1 ) by alloying the cyclic organic amine 3-hydroxypyridine. 1 displays a remarkable switchable dielectric response induced by an order-disorder transformation of the organic moiety, this transformation behaviour is confirmed by DSC and Hirshfeld surface measurements. More interestingly, 1 has a narrowband emission (FWHM=4.64 nm) at 590 nm; FWHM is a major quality figure for narrowband photodetectors. In addition, 1 exhibits semiconducting properties with an indirect bandgap of 2.78 eV by the analysis of the UV-Vis absorption results.     

Comparative Analysis of Hydration Layer Reorientation Dynamics of Antifreeze Protein and Protein Cytochrome P450

Antifreeze proteins (AFPs) inhibit ice recrystallization by a mechanism remaining largely elusive. Dynamics of AFPs' hydration water and its involvement in the antifreeze activity have not been identified conclusively. We herein, by simulation and theory, examined the water reorientation dynamics in the first hydration layer of an AFP from the spruce budworm, Choristoneura fumiferana, compared with a protein cytochrome P450 (CYP). The increase of potential acceptor water molecules around donor water molecules leads to the acceleration of hydrogen bond exchange between water molecules. Therefore, the jump reorientation of water molecules around the AFP active region is accelerated. Due to the mutual coupling and excitation of hydrogen bond exchange, with the acceleration of hydrogen bond exchange, the rearrangement of the hydrogen bond network and the frame reorientation of water are accelerated. Therefore, the water reorientation dynamics of AFP is faster than that of CYP. The results of this study provide a new physical image of antifreeze protein and a new understanding of the antifreeze mechanism of antifreeze proteins.     

基于压缩感知的动态散射成像

利用基于压缩感知的成像系统可以透过静态的散射介质获得高质量的重建图像. 但是当散射介质动态变化时, 因为采样所得的测量值受到散射介质衰减系数非线性变化的影响, 重建图像质量会大大下降. 针对上述情况, 本文提出基于压缩感知成像系统的测量值线性拉伸算法, 该算法能够对所得到的非线性测量值进行分析, 根据测量值大小的不同将测量值划分成数个区域并计算补偿系数, 从而根据补偿系数进行测量值线性拉伸变换, 使测量值线性化. 最后再对变换后的测量值进行压缩感知重建计算. 通过理论分析、计算机仿真和实验证明了所提算法能够有效地应对动态的散射介质, 提高基于压缩感知成像系统在透过动态散射介质时的图像重建质量.     

Pulse advancement and delay in an integrated-optical two-port ring-resonator circuit: direct experimental observations

We report experimental observations of the negative-group-velocity (v(g)) phenomenon in an integrated-optical two-port ring-resonator circuit. We demonstrate that when the v(g) is negative, the (main) peak of output pulse appears earlier than the peak of a reference pulse, while for a positive v(g), the situation is the other way around. We observed that a pulse splitting phenomenon occurs in the neighborhood of the critical-coupling point. This pulse splitting limits the maximum achievable delay and advancement of a single device as well as facilitating a smooth transition from highly advanced to highly delayed pulse, and vice versa, across the critical-coupling point.