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41.
Laurens Kooijman Dr. Matthias Schuster Christian Baumann Simon Jurt Dr. Frank Löhr Dr. Boris Fürtig Prof. Dr. Peter Güntert Prof. Dr. Oliver Zerbe 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(47):21151-21158
To achieve efficient proton pumping in the light-driven proton pump bacteriorhodopsin (bR), the protein must be tightly coupled to the retinal to rapidly convert retinal isomerization into protein structural rearrangements. Methyl group dynamics of bR embedded in lipid nanodiscs were determined in the dark-adapted state, and were found to be mostly well ordered at the cytosolic side. Methyl groups in the M145A mutant of bR, which displays only 10 % residual proton pumping activity, are less well ordered, suggesting a link between side-chain dynamics on the cytosolic side of the bR cavity and proton pumping activity. In addition, slow conformational exchange, attributed to low frequency motions of aromatic rings, was indirectly observed for residues on the extracellular side of the bR cavity. This may be related to reorganization of the water network. These observations provide a detailed picture of previously undescribed equilibrium dynamics on different time scales for ground-state bR. 相似文献
42.
Dr. Chenge Li Dr. Alison G. Tebo Marion Thauvin Marie-Aude Plamont Prof. Dr. Michel Volovitch Dr. Xavier Morin Prof. Dr. Sophie Vriz Prof. Dr. Arnaud Gautier 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(41):18073-18079
Far-red emitting fluorescent labels are highly desirable for spectral multiplexing and deep tissue imaging. Here, we describe the generation of frFAST (far-red Fluorescence Activating and absorption Shifting Tag), a 14-kDa monomeric protein that forms a bright far-red fluorescent assembly with (4-hydroxy-3-methoxy-phenyl)allylidene rhodanine (HPAR-3OM). As HPAR-3OM is essentially non-fluorescent in solution and in cells, frFAST can be imaged with high contrast in presence of free HPAR-3OM, which allowed the rapid and efficient imaging of frFAST fusions in live cells, zebrafish embryo/larvae, and chicken embryos. Beyond enabling the genetic encoding of far-red fluorescence, frFAST allowed the design of a far-red chemogenetic reporter of protein–protein interactions, demonstrating its great potential for the design of innovative far-red emitting biosensors. 相似文献
43.
In this work, a vanillin complex is immobilized onto MCM-41 and characterized by FT-IR, X-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, thermogravimetric analysis, and BET techniques. This supported Schiff base complex was found to be an efficient and recoverable catalyst for the chemoselective oxidation of sulfides into sulfoxides and thiols into their corresponding disulfides (using hydrogen peroxide as a green oxidant) and also a suitable catalyst for the preparation of 2,3-dihydroquinazolin-4(1H)-one derivatives in water at 90°C. Using this protocol, we show that a variety of disulfides, sulfoxides, and 2,3-dihydroquinazolin-4(1H)-one derivatives can be synthesized in green conditions. The catalyst can be recovered and recycled for further reactions without appreciable loss of catalytic performance. 相似文献
44.
The Swendsen‐Wang (SW) dynamics is a popular Markov chain for sampling from the Gibbs distribution for the ferromagnetic Ising model on a graph G = (V,E). The dynamics is conjectured to converge to equilibrium in O(|V|1/4) steps at any (inverse) temperature β, yet there are few results providing o(|V|) upper bounds. We prove fast convergence of the SW dynamics on general graphs in the tree uniqueness region. In particular, when β < βc(d) where βc(d) denotes the uniqueness/nonuniqueness threshold on infinite d‐regular trees, we prove that the relaxation time (i.e., the inverse spectral gap) of the SW dynamics is Θ(1) on any graph of maximum degree d ≥ 3. Our proof utilizes a monotone version of the SW dynamics which only updates isolated vertices. We establish that this variant of the SW dynamics has mixing time and relaxation time Θ(1) on any graph of maximum degree d for all β < βc(d). Our proof technology can be applied to general monotone Markov chains, including for example the heat‐bath block dynamics, for which we obtain new tight mixing time bounds. 相似文献
45.
Artem Yakovliev Tymish Y. Ohulchanskyy Roman Ziniuk Tereza Dias Xin Wang Hao Xu Guanying Chen Junle Qu Anderson S. L. Gomes 《Particle & Particle Systems Characterization》2020,37(2):1900445
In this work, the application of near infrared (NIR)-emitting NaYbF4:1%Tm3+@NaLuF4:30%Nd3+ core–shell nanoparticles is reported for noninvasive probing and monitoring the temperature during photopolymerization of dental materials. When excited at 808 nm, the synthesized nanoparticles emit NIR photoluminescence (PL) with two distinctive peaks at 865 and 980 nm which correspond to radiative transitions from the doped Nd3+ and Yb3+ ions, respectively. Luminescence intensity ratio between these two bands is found to vary with temperature due to temperature-dependent electronic excitation energy transfer between Nd3+ and Yb3+ ions at the core/shell interface. This finding allows luminescence ratiometric evaluation of the in situ temperature during photopolymerization of resin cement (doped with nanoparticles) in a veneer placement procedure. In addition, the NIR emission also enables PL imaging of the distribution of the adhesive under the veneer. The results highlight that rare-earth ions–doped nanoparticles with both excitation and emission in the NIR spectral range are advantageous for both PL-based nanothermometry and imaging due to the reduced attenuation of NIR light by dental ceramics. 相似文献
46.
酸性环境引发的岩石孔隙表面溶解增加了孔隙内水溶液的盐离子浓度,破坏了孔隙的表面结构.本文采用分子动力学模拟的方法研究了纳米级岩石孔隙内水溶液的流动特性,分析了盐离子浓度和孔隙表面结构对水流速度分布的影响及原因.研究结果表明:纳米级岩石孔隙内的水溶液流动符合泊肃叶流动特性,流速呈"抛物线"分布;随盐离子浓度增加,水溶液内部氢键网络变得更为致密,水黏度随其呈线性增长;水溶液中离子浓度越大,孔隙表面对水流动的阻力越大,最大流速越小,速度分布的"抛物线"曲率半径越大;岩石孔隙表面结构的破坏改变了流动表面的粗糙程度,增加了孔隙表面对H2O分子的吸引力.随表面结构破坏程度的增大,水溶液在近壁区域的密度增大,流速降低;当表面破坏程度达到50%时,水溶液在近壁区域出现了明显的负边界滑移现象. 相似文献
47.
We examined the flow behaviors and mixing characteristics of double-concentric jets using laser-assisted smoke flow visualization method to analyze typical flow patterns and binary boundary detection technique to investigate jet spread width. Time-averaged velocity vectors, streamline patterns, velocity distributions, turbulence properties, and vorticity contours were analyzed using Particle Image Velocimetry (PIV). Topological flow patterns were analyzed to interpret the vortical flow structures. Mixing properties were investigated using a tracer-gas concentration detection method. Four characteristic modes were observed: annular flow dominated mode, transition mode, central jet dominated mode-low shear, and central jet dominated mode-high shear. The jets’ mixing properties were enhanced by two major phenomena: the merging of annular flow and central jet at the centerline and the large turbulence fluctuations produced in the flow field. The merging of the jets induced stagnation points on the central axis in the annular flow dominated mode, which caused reverse flow on the central axis and drastic turbulence fluctuations of the near field region. When the central jet penetrated the recirculation region in the other three modes, the stagnation points on the central axis and the reverse flow vanished. Therefore, the mixing behaviors were prominently enhanced in the annular flow dominated mode. 相似文献
48.
A theoretical model of an elastic panel in hypersonic flow is derived to be used for design and analysis. The nonlinear von Kármán plate equations are coupled with 1st order Piston Theory and linearized at the nonlinear steady-state deformation due to static pressure differential and thermal loads. Eigenvalue analysis is applied to determine the system’s stability, natural frequencies and mode shapes. Numerically time marching the equations provides transient response prediction which can be used to estimate limit cycle oscillation amplitude, frequency and time to onset. The model’s predictive capability is assessed by comparison to an experiment conducted at a free stream flow of Mach 6. Good agreement is shown between the theoretical and experimental natural frequencies and mode shapes of the fluid–structure system. Stability analysis is performed using linear and nonlinear methods to plot stability, flutter and buckling zones on a free stream static pressure vs temperature differential plane. 相似文献
49.
针对现有成像系统因数据冗余而无法兼顾大视场、高分辨、高效性的问题,结合人眼视网膜变分辨成像和并列式复眼成像原理,设计一种多分辨率成像的复合仿生成像系统.该成像系统按照球面和平面兼顾的曲面布局方式,利用11个相机镜头构建相机阵列,组成了四个等级分辨率的子眼拍摄模块.通过物距100 m的远景实验和物距10 m的近景实验发现,该系统在实现高分辨成像的同时,获得总视场达150.8°×37.8°.多分辨率成像实验结果表明,该系统获取的图像的分辨率从中心视场到边缘视场逐渐降低,并且相较于中心清晰全视场成像,四级分辨率成像的拼接图像数据量减少了17.2倍的数据冗余. 相似文献
50.
针对空中目标在复杂背景下的探测需求,根据实际目标的运动特性,分析目标在飞行高度、飞行姿态角改变时的辐射特点,基于MODTRAN计算得到大气辐射和衰减数据,建立目标的三维模型、热辐射和反射模型,搭建空中目标的红外成像仿真系统.分析和仿真结果表明:在中波波段,目标尾焰的红外辐射比蒙皮强很多,在长波波段,蒙皮的红外辐射比较强,仿真图像的细节比较多,尾焰的红外辐射虽然有所减弱,红外成像效果依旧很好;相同探测条件下,由于位置越高大气越稀薄,探测器的可探测距离会变得比较远.目标红外辐射特性的分析和红外仿真系统的搭建对缩短红外探测器的研制周期和进一步确定探测器波段和系统分辨率等指标提供了参考依据. 相似文献