共查询到20条相似文献，搜索用时 78 毫秒
1.
Kim M Hohman JN Cao Y Houk KN Ma H Jen AK Weiss PS 《Science (New York, N.Y.)》2011,331(6022):1312-1315
The products of photoreactions of conjugated organic molecules may be allowed by selection rules but not observed in solution reactions because of unfavorable reaction geometries. We have used defect sites in self-assembled alkanethiolate monolayers on gold surfaces to direct geometrically unfavorable photochemical reactions between individual organic molecules. High conductivity and stochastic switching of anthracene-terminated phenylethynylthiolates within alkanethiolate monolayers, as well as in situ photochemical transformations, have been observed and distinguished with the scanning tunneling microscope (STM). Ultraviolet light absorbed during imaging increases the apparent heights of excited molecules in STM images, a direct manifestation of probing electronically excited states. 相似文献
2.
Lahann J Mitragotri S Tran TN Kaido H Sundaram J Choi IS Hoffer S Somorjai GA Langer R 《Science (New York, N.Y.)》2003,299(5605):371-374
We report the design of surfaces that exhibit dynamic changes in interfacial properties, such as wettability, in response to an electrical potential. The change in wetting behavior was caused by surface-confined, single-layered molecules undergoing conformational transitions between a hydrophilic and a moderately hydrophobic state. Reversible conformational transitions were confirmed at a molecular level with the use of sum-frequency generation spectroscopy and at a macroscopic level with the use of contact angle measurements. This type of surface design enables amplification of molecular-level conformational transitions to macroscopic changes in surface properties without altering the chemical identity of the surface. Such reversibly switching surfaces may open previously unknown opportunities in interfacial engineering. 相似文献
3.
Angstrom-resolution atomic force microscope images of Langmuir-Blodgett monolayers and multilayers of cadmium arachidate in air and under water show a dramatic change from a disordered arrangement to a crystalline lattice by the addition or removal of a single layer of molecules. The disordered surface is less stable than the ordered one to mechanical stresses such as atomic force microscopy tip forces or at the air-water contact line during contact angle measurements. The difference in the degree of order in the alkyl chains is attributed to the strong attractive interaction between headgroups in the presence of the divalent cation. 相似文献
4.
Interfacial force microscopy has been used to show that a single layer of self-assembling molecules adsorbed on a gold substrate can prevent adhesion between gold and a tungsten probe. The passivated gold is able to elastically support large repulsive loads, with plots of load versus deformation closely following the Hertzian model. The gold shear-stress threshold for plastic deformation is determined to be approximately 1 gigapascal, which is in agreement with the theoretical value for the intrinsic gold-lattice stability. 相似文献
5.
Molecular dynamics simulations and atomic force microscopy are used to investigate the atomistic mechanisms of adhesion, contact formation, nanoindentation, separation, and fracture that occur when a nickel tip interacts with a gold surface. The theoretically predicted and experimentally measured hysteresis in the force versus tip-to-sample distance relationship, found upon approach and subsequent separation of the tip from the sample, is related to inelastic deformation of the sample surface characterized by adhesion of gold atoms to the nickel tip and formation of a connective neck of atoms. At small tipsample distances, mechanical instability causes the tip and surface to jump-to-contact, which in turn leads to adhesion-induced wetting of the nickel tip by gold atoms. Subsequent indentation of the substrate results in the onset of plastic deformation of the gold surface. The atomic-scale mechanisms underlying the formation and elongation of a connective neck, which forms upon separation, consist of structural transformations involving elastic and yielding stages. 相似文献
6.
The bistability in the position of the two hydrogen atoms in the inner cavity of single free-base naphthalocyanine molecules constitutes a two-level system that was manipulated and probed by low-temperature scanning tunneling microscopy. When adsorbed on an ultrathin insulating film, the molecules can be switched in a controlled fashion between the two states by excitation induced by the inelastic tunneling current. The tautomerization reaction can be probed by resonant tunneling through the molecule and is expressed as considerable changes in the conductivity of the molecule. We also demonstrated a coupling of the switching process so that the charge injection in one molecule induced tautomerization in an adjacent molecule. 相似文献
7.
By trapping molecules between two gold electrodes with a temperature difference across them, the junction Seebeck coefficients of 1,4-benzenedithiol (BDT), 4,4'-dibenzenedithiol, and 4,4'-tribenzenedithiol in contact with gold were measured at room temperature to be +8.7 +/- 2.1 microvolts per kelvin (muV/K), +12.9 +/- 2.2 muV/K, and +14.2 +/- 3.2 muV/K, respectively (where the error is the full width half maximum of the statistical distributions). The positive sign unambiguously indicates p-type (hole) conduction in these heterojunctions, whereas the Au Fermi level position for Au-BDT-Au junctions was identified to be 1.2 eV above the highest occupied molecular orbital level of BDT. The ability to study thermoelectricity in molecular junctions provides the opportunity to address these fundamental unanswered questions about their electronic structure and to begin exploring molecular thermoelectric energy conversion. 相似文献
8.
Weisenhorn AL Mac Dougall JE Gould SA Cox SD Wise WS Massie J Maivald P Elings VB Stucky GD Hansma PK 《Science (New York, N.Y.)》1990,247(4948):1330-1333
The adsorption of neutral molecules and ions on the surfaces of zeolites was observed in real time with an atomic force microscope (AFM). Direct imaging of the surface of the zeolite clinoptilolite was possible by using a diluted tert-butyl ammonium chloride solution as a medium. Images of the crystal in different liquids revealed that molecules could be bound to the surface in different ways; neutral molecules of tert-butanol formed an ordered array, whereas tert-butyl ammonium ions formed clusters. These absorbed molecules were not rearranged by the AFM tip when used in an imaging mode. However, when a sufficiently large force was applied, the tip of the AFM could rearrange the tert-butyl ammonium ions on the zeolite surface. This demonstration of molecular manipulation suggests new applications, including biosensors and lithography. 相似文献
9.
确定叠梁层间发生接触的区间及接触力分布规律是叠梁计算的关键.为克服以往解析解答得到的结论不合实际的现象，将叠梁接触问题构造为线性互补问题，并给出其一般求解过程.为验证该法的合理性，以梁与刚体接触问题的Timoshenko解答与胡海昌解答为例进行对比分析.在此基础上，对典型荷载作用下的叠梁接触问题进行了计算，并对其影响因素进行了深入研究.最后得到如下主要结论：刚度比、荷载作用形式以及剪切挠度对叠梁层间接触规律影响均非常明显；考虑剪切变形影响时，叠梁接触力由集中力变为分布力；集中力作用下，叠梁接触趋于点接触，均布力作用下，叠梁接触趋于线接触；上下梁刚度相等是叠梁接触力分布规律的一个转折点，不同的上下梁刚度比会得到不同的接触规律. 相似文献
10.
Yoshida H Kuwauchi Y Jinschek JR Sun K Tanaka S Kohyama M Shimada S Haruta M Takeda S 《Science (New York, N.Y.)》2012,335(6066):317-319
Understanding how molecules can restructure the surfaces of heterogeneous catalysts under reaction conditions requires methods that can visualize atoms in real space and time. We applied a newly developed aberration-corrected environmental transmission electron microscopy to show that adsorbed carbon monoxide (CO) molecules caused the {100} facets of a gold nanoparticle to reconstruct during CO oxidation at room temperature. The CO molecules adsorbed at the on-top sites of gold atoms in the reconstructed surface, and the energetic favorability of this reconstructed structure was confirmed by ab initio calculations and image simulations. This atomic-scale visualizing method can be applied to help elucidate reaction mechanisms in heterogeneous catalysis. 相似文献
11.
Recent developments in piconewton instrumentation allow the manipulation of single molecules and measurements of intermolecular as well as intramolecular forces. Dextran filaments linked to a gold surface were probed with the atomic force microscope tip by vertical stretching. At low forces the deformation of dextran was found to be dominated by entropic forces and can be described by the Langevin function with a 6 angstrom Kuhn length. At elevated forces the strand elongation was governed by a twist of bond angles. At higher forces the dextran filaments underwent a distinct conformational change. The polymer stiffened and the segment elasticity was dominated by the bending of bond angles. The conformational change was found to be reversible and was corroborated by molecular dynamics calculations. 相似文献
12.
湖羊GHR和IGF-Ⅰ基因表达的发育性变化 及其与肉质性状的关联 总被引：1，自引：1，他引：0
【目的】探讨生长激素受体（growth hormone receptor,GHR）和胰岛素样生长因子-Ⅰ（insulin-like growth factor-Ⅰ,IGF-Ⅰ）基因在湖羊不同生长阶段背最长肌中表达丰度与肉质性能的相关性以及这两个基因表达水平的关联性,为湖羊肌肉生长性状的选育提供遗传学资料。【方法】利用荧光定量RT-PCR分析GHR和IGF-Ⅰ基因在湖羊早期生长背最长肌肉组织中的mRNA的发育性变化。【结果】①出生后随着月龄的增加,母羊GHR基因在背最长肌的表达趋势为：先升高后降低再升高再降低最后再升高,最后6月龄到达最高点;公羊GHR在背最长肌的表达趋势为：先升高到2月龄到达一个峰值,2月龄到4月龄为一个降低的过程,4月龄到6月龄又升高,并到达最高点;母羊IGF-Ⅰ基因在背最长肌的表达趋势为：由2日龄开始依次升高最后于6月龄到达最高点;公羊IGF-Ⅰ基因在背最长肌的表达趋势为：先升高到1月龄到达一个峰值,1月龄到3月龄为一个降低的过程,并于3月龄降至与初生接近相等的水平,此后随月龄增加逐渐升高,并于6月龄到达最高点;②GHR和IGF-Ⅰ基因在湖羊各月龄间大多存在显著或极显著差异,湖羊的公羊和母羊的GHR和IGF-Ⅰ基因的相同生长阶段的表达也大多存在显著或极显著差异;③GHR和IGF-Ⅰ基因的表达存在显著正相关（0.01＜P＜0.05）,GHRI和GF-I基因与肌纤维直径均存在极显著正相关（P＜0.01）,GHR与肌纤剪切力存在极显著正相关（P＜0.01）,IGF-Ⅰ与肌纤剪切力存在显著正相关（0.01＜P＜0.05）,GHR和IGF-Ⅰ基因与肌纤维密度均存在极显著负相关（P＜0.01）。【结论】性别和年龄对于GHR和IGF-Ⅰ基因在湖羊不同生长阶段的肌肉中的表达具有重要影响;出生后,各基因表达水平并非随之上升或者下降,各基因表达水平出现拐点的时间并不相同;GHR和IGF-Ⅰ基因在湖羊早期肌肉性状的表达为显著正相关,可以作为湖羊早期肉质性状的候选基因。 相似文献
13.
Computer simulations of hydrocarbon and related molecules using empirical force fields have become important tools for studying a number of biological and related processes at the atomic scale. Traditional force fields, however, cannot be used to simulate dynamic chemical reactivity that involves changes in atomic hybridization. Application of a many-body potential function allows such reactivity to occur in a computer simulation. Simulations of the reaction of small hydrocarbon molecules adsorbed on a reconstructed diamond {001}(2x1) surface suggest that these hydrocarbons are highly reactive species and that initial stages of diamond growth proceed through a dimer-opening mechanism. Rates estimated from transition state theory of two interconversions between states where the dimer is open and closed are given. 相似文献
14.
Sirringhaus H Kawase T Friend RH Shimoda T Inbasekaran M Wu W Woo EP 《Science (New York, N.Y.)》2000,290(5499):2123-2126
Direct printing of functional electronic materials may provide a new route to low-cost fabrication of integrated circuits. However, to be useful it must allow continuous manufacturing of all circuit components by successive solution deposition and printing steps in the same environment. We demonstrate direct inkjet printing of complete transistor circuits, including via-hole interconnections based on solution-processed polymer conductors, insulators, and self-organizing semiconductors. We show that the use of substrate surface energy patterning to direct the flow of water-based conducting polymer inkjet droplets enables high-resolution definition of practical channel lengths of 5 micrometers. High mobilities of 0.02 square centimeters per volt second and on-off current switching ratios of 10(5) were achieved. 相似文献
15.
Small metal particles (<5 nanometers), which are widely used in catalysis, have physical and chemical properties that are markedly different from those of the bulk metal. The differences are related to crystal structure, and it is therefore significant that structral rearrangements in small particles have been observed in real time by using high-resolution electron microscopy. A detailed investigation at the atomic level has been made of the factors affecting the dynamic activity of small gold crystals that are supported on thin films of amorphous carbon, silicon, and germanium. The rate of activity depends mainly on the current density of the incident electron beam and the degree of contact of the particle with the substrate, but this rate decreases rapidly as the particle size is increased. The activity of the particles is very similar on either carbon or silicon, but it is generally less marked on germanium because of increased contact between the particle and the substrate. The electron beam effectively heats the particles, and it appears that their dynamic behavior depends on their thermal contact with the substrate. 相似文献
16.
Igarashi K Uchihashi T Koivula A Wada M Kimura S Okamoto T Penttilä M Ando T Samejima M 《Science (New York, N.Y.)》2011,333(6047):1279-1282
A deeper mechanistic understanding of the saccharification of cellulosic biomass could enhance the efficiency of biofuels development. We report here the real-time visualization of crystalline cellulose degradation by individual cellulase enzymes through use of an advanced version of high-speed atomic force microscopy. Trichoderma reesei cellobiohydrolase I (TrCel7A) molecules were observed to slide unidirectionally along the crystalline cellulose surface but at one point exhibited collective halting analogous to a traffic jam. Changing the crystalline polymorphic form of cellulose by means of an ammonia treatment increased the apparent number of accessible lanes on the crystalline surface and consequently the number of moving cellulase molecules. Treatment of this bulky crystalline cellulose simultaneously or separately with T. reesei cellobiohydrolase II (TrCel6A) resulted in a remarkable increase in the proportion of mobile enzyme molecules on the surface. Cellulose was completely degraded by the synergistic action between the two enzymes. 相似文献
17.
【目的】实现番木瓜稳定无损伤摘取。【方法】采用三指对称夹持后扭断的摘取方案,构建摘取接触力平衡方程,依据三指内力汇交原理进行抓取稳定性分析,制定摘取接触力学模型求解方案,并对番木瓜进行摘取试验。【结果】样本表面无明显变形、压痕与裂纹,夹持处果肉室温静置24 h后无明显的颜色变化和伤痕,最大夹持力远小于成熟番木瓜横径方向受压弹性变形阶段压力极限值;质量和摘取扭转力矩与横径、纵径、果柄长度、果柄扭断直径有密切依存关系,质量多元线性回归达极显著水平,扭转力矩多元线性回归达显著水平;依据接触力学模型和回归模型计算的理论夹持力与测量夹持力对比,测量夹持力均高于理论夹持力,两者最大偏差小于20%,两者在趋势上具有较好一致性。【结论】摘取方案能稳定无损伤摘取番木瓜,摘取接触力学模型具有正确性与实用性,可为番木瓜摘取末端执行机构设计与力度控制提供依据。 相似文献
18.
J F Hainfeld 《Science (New York, N.Y.)》1987,236(4800):450-453
A general method has been developed to make the smallest gold-conjugated antibody label yet developed for electron microscopy. It should have wide application in domainal mapping of single molecules or in pinpointing specific molecules, sites, or sequences in supramolecular complexes. It permits electron microscopic visualization of single antigen-binding antibody fragments (Fab') by covalently linking an 11-atom gold cluster to a specific residue on each Fab' such that the antigenic specificity and capacity are preserved. The distance of the gold cluster from the antigen is a maximum of 5.0 nanometers when the undecagold-Fab' probe is used as an immunolabel. 相似文献
19.
"Dip-Pen" nanolithography 总被引：1，自引：0，他引：1
A direct-write "dip-pen" nanolithography (DPN) has been developed to deliver collections of molecules in a positive printing mode. An atomic force microscope (AFM) tip is used to write alkanethiols with 30-nanometer linewidth resolution on a gold thin film in a manner analogous to that of a dip pen. Molecules are delivered from the AFM tip to a solid substrate of interest via capillary transport, making DPN a potentially useful tool for creating and functionalizing nanoscale devices. 相似文献
20.
Soft lithography is an alternative to silicon-based micromachining that uses replica molding of nontraditional elastomeric materials to fabricate stamps and microfluidic channels. We describe here an extension to the soft lithography paradigm, multilayer soft lithography, with which devices consisting of multiple layers may be fabricated from soft materials. We used this technique to build active microfluidic systems containing on-off valves, switching valves, and pumps entirely out of elastomer. The softness of these materials allows the device areas to be reduced by more than two orders of magnitude compared with silicon-based devices. The other advantages of soft lithography, such as rapid prototyping, ease of fabrication, and biocompatibility, are retained. 相似文献