Functionalizing hydrogen-bonded surface networks with self-assembled monolayers

One of the central challenges in nanotechnology is the development of flexible and efficient methods for creating ordered structures with nanometre precision over an extended length scale. Supramolecular self-assembly on surfaces offers attractive features in this regard: it is a 'bottom-up' approach and thus allows the simple and rapid creation of surface assemblies, which are readily tuned through the choice of molecular building blocks used and stabilized by hydrogen bonding, van der Waals interactions, pi-pi bonding or metal coordination between the blocks. Assemblies in the form of two-dimensional open networks are of particular interest for possible applications because well-defined pores can be used for the precise localization and confinement of guest entities such as molecules or clusters, which can add functionality to the supramolecular network. Another widely used method for producing surface structures involves self-assembled monolayers (SAMs), which have introduced unprecedented flexibility in our ability to tailor interfaces and generate patterned surfaces. But SAMs are part of a top-down technology that is limited in terms of the spatial resolution that can be achieved. We therefore rationalized that a particularly powerful fabrication platform might be realized by combining non-covalent self-assembly of porous networks and SAMs, with the former providing nanometre-scale precision and the latter allowing versatile functionalization. Here we show that the two strategies can indeed be combined to create integrated network-SAM hybrid systems that are sufficiently robust for further processing. We show that the supramolecular network and the SAM can both be deposited from solution, which should enable the widespread and flexible use of this combined fabrication method.     

Complex shapes self-assembled from single-stranded DNA tiles

Programmed self-assembly of strands of nucleic acid has proved highly effective for creating a wide range of structures with desired shapes. A particularly successful implementation is DNA origami, in which a long scaffold strand is folded by hundreds of short auxiliary strands into a complex shape. Modular strategies are in principle simpler and more versatile and have been used to assemble DNA or RNA tiles into periodic and algorithmic two-dimensional lattices, extended ribbons and tubes, three-dimensional crystals, polyhedra and simple finite two-dimensional shapes. But creating finite yet complex shapes from a large number of uniquely addressable tiles remains challenging. Here we solve this problem with the simplest tile form, a 'single-stranded tile' (SST) that consists of a 42-base strand of DNA composed entirely of concatenated sticky ends and that binds to four local neighbours during self-assembly. Although ribbons and tubes with controlled circumferences have been created using the SST approach, we extend it to assemble complex two-dimensional shapes and tubes from hundreds (in some cases more than one thousand) distinct tiles. Our main design feature is a self-assembled rectangle that serves as a molecular canvas, with each of its constituent SST strands--folded into a 3 nm-by-7 nm tile and attached to four neighbouring tiles--acting as a pixel. A desired shape, drawn on the canvas, is then produced by one-pot annealing of all those strands that correspond to pixels covered by the target shape; the remaining strands are excluded. We implement the strategy with a master strand collection that corresponds to a 310-pixel canvas, and then use appropriate strand subsets to construct 107 distinct and complex two-dimensional shapes, thereby establishing SST assembly as a simple, modular and robust framework for constructing nanostructures with prescribed shapes from short synthetic DNA strands.     

Evolution of cooperative strategies from first principles

One of the greatest challenges in the modern biological and social sciences is to understand the evolution of cooperative behaviour. General outlines of the answer to this puzzle are currently emerging as a result of developments in the theories of kin selection, reciprocity, multilevel selection and cultural group selection. The main conceptual tool used in probing the logical coherence of proposed explanations has been game theory, including both analytical models and agent-based simulations. The game-theoretic approach yields clear-cut results but assumes, as a rule, a simple structure of payoffs and a small set of possible strategies. Here we propose a more stringent test of the theory by developing a computer model with a considerably extended spectrum of possible strategies. In our model, agents are endowed with a limited set of receptors, a set of elementary actions and a neural net in between. Behavioural strategies are not predetermined; instead, the process of evolution constructs and reconstructs them from elementary actions. Two new strategies of cooperative attack and defence emerge in simulations, as well as the well-known dove, hawk and bourgeois strategies. Our results indicate that cooperative strategies can evolve even under such minimalist assumptions, provided that agents are capable of perceiving heritable external markers of other agents.     

Improved photostability of Vitamin A palmitate originating from self-assembled supramolecular gels

Retinyl palmitate(RP) is a derivative of Vitamin A and widely applied as the active component in the fields of cosmetic and pharmaceutics.RP can easily lose its physiological activity under UV irradiation due to its photosensitivity.In this work,it was found that the activity of RP remained 75% after 80 min of UVA irradiation when RP was entrapped in supramolecular gels formed by self-assembly of sorbitol-based gelators.By contrast,the activity of RP in conventional hydroxyethyl cellulose gels only remained 10% under the same conditions.These results showed that the supramolecular gels exhibited a significant protective effect on the photostability of RP.UV spectra of RP in supramolecular gels and corresponding solutions showed no distinct differences,indicating no change of the physicochemical properties of RP.The images of field-emission scanning electron microscopy and fluorescent optical microscopy suggested that the protection by supramolecular gels on the photostability of RP may be attributed to the three-dimensional network structure formed by the self-assembly of the gelators,which reduced the molecular collisions and the degradation process of the photoactivated RP.The present results showed that this protection can be influenced by the structures and the concentration of gelators as well as by the solvent composition.     

从违反合作原则看会话含义

为了保证会话的顺利进行,谈话双方必须共同遵守一些基本原则,这就是格莱斯的“合作原则”。本文阐述了合作原则的四条准则,分析了违反这些准则所产生的会话含义。     

螺旋结构的曲率和挠率分析及其在工艺上的应用

研究自然界的螺旋现象夏其在工艺上的运用．利用微分几何的曲率、挠率及广义相对论的理论知识分析了螺旋形结构,指出自然选择这种螺旋结构的益处,探讨了螺旋造型的一些奥秘,并给出其在工艺上的一些应用例子．     

螺带螺杆搅拌釜中高黏流体的CFD模拟计算

高黏聚合体系的搅拌混合应用广泛,是聚合物合成工业中的关键,但采用实验方法难以得到其流场.应用ANSYS CFX软件模拟计算高黏聚苯乙烯溶液体系在不同螺带螺杆组合搅拌釜中的流场特征,分别采用不同的计算流场模型进行求解,其中搅拌釜气-液两相界面采用与实际情况较为接近的自由液面,旋转区域采用滑移网格法处理,液相采用不同黏度的高分子黏性流体,计算比较了不同搅拌桨组合下的流场特征,论证了双螺带螺杆搅拌桨在高黏流体混合中的优越性,同时得到不同黏度和不同转速下搅拌釜内的液面形状、速度场和搅拌功率,为实际生产及工业优化提供了理论参考.     

混合顺序作业堆场BAY优化模型

介绍了集装箱堆场优化的重要意义,提出了混合顺序堆场作业的概念,在图搜索技术和模式识别理论的基础上建立了随机条件下的混合顺序作业堆场ＢＡＹ优化模型,计算机模拟结果证明：混合顺序作业堆场ＢＡＹ优化模型可以在堆场作业不倒箱的情况下,产生符合配载要求的堆场。     

Experimental extraction of an entangled photon pair from two identically decohered pairs

Entanglement is considered to be one of the most important resources in quantum information processing schemes, including teleportation, dense coding and entanglement-based quantum key distribution. Because entanglement cannot be generated by classical communication between distant parties, distribution of entangled particles between them is necessary. During the distribution process, entanglement between the particles is degraded by the decoherence and dissipation processes that result from unavoidable coupling with the environment. Entanglement distillation and concentration schemes are therefore needed to extract pairs with a higher degree of entanglement from these less-entangled pairs; this is accomplished using local operations and classical communication. Here we report an experimental demonstration of extraction of a polarization-entangled photon pair from two decohered photon pairs. Two polarization-entangled photon pairs are generated by spontaneous parametric down-conversion and then distributed through a channel that induces identical phase fluctuations to both pairs; this ensures that no entanglement is available as long as each pair is manipulated individually. Then, through collective local operations and classical communication we extract from the two decohered pairs a photon pair that is observed to be polarization-entangled.     

Chemically tailorable colloidal particles from infinite coordination polymers

Micrometre- and nanometre-sized particles play important roles in many applications, including catalysis, optics, biosensing and data storage. Organic particles are usually prepared through polymerization of suitable monomers or precipitation methods. In the case of inorganic materials, particle fabrication tends to involve the reduction of a metal salt, or the controlled mixing of salt solutions supplying a metal cation and an elemental anion (for example, S2-, Se2-, O2-), respectively; in some instances, these methods even afford direct control over the shape of the particles produced. Another class of materials are metal-organic coordination polymers, which are based on metal ions coordinated by polydentate organic ligands and explored for potential use in catalysis, gas storage, nonlinear optics and molecular recognition and separations. In a subset of these materials, the use of organometallic complexes as ligands (so-called metalloligands) provides an additional level of tailorability, but these materials have so far not yet been fashioned into nano- or microparticles. Here we show that simple addition of an initiation solvent to a precursor solution of metal ions and metalloligands results in the spontaneous and fully reversible formation of a new class of metal-metalloligand particles. We observe initial formation of particles with diameters of a few hundred nanometres, which then coalesce and anneal into uniform and smooth microparticles. The ease with which these particles can be fabricated, and the ability to tailor their chemical and physical properties through the choice of metal and organic ligand used, should facilitate investigations of their scope for practical applications.     

氢键系统中质子传递的孤子特性

用庞小峰先生提出的氢键系统的非线性激发与质子传递的新理论并采用四阶Runge-Kutta数值分析方法,通过计算机模拟,研究了冰晶体中质子传递孤子的动力学特征.研究表明,该孤子在传递过程中状态一直保持稳定,能够较好的实验结果符合.从而自数值模拟角度证明了新理论的可利用性.     

Charting a course for genomic medicine from base pairs to bedside

There has been much progress in genomics in the ten years since a draft sequence of the human genome was published. Opportunities for understanding health and disease are now unprecedented, as advances in genomics are harnessed to obtain robust foundational knowledge about the structure and function of the human genome and about the genetic contributions to human health and disease. Here we articulate a 2011 vision for the future of genomics research and describe the path towards an era of genomic medicine.     

氢键系统中弧子偶的传递特性

运用能量分析方法,研究了在外场、阻尼和随机力作用下,氢键系统中的非线性激发和孤子偶的传递特性,推导了孤子偶能量和有效质量的表达式,讨论了热孤子偶的核化规律,计算了孤子偶的电导率,理论结果与实验相一致.     

螺旋结构与旋光方向V—1，2—二取代与二茂铁类分子的螺旋结构与旋光方向

阐述了1,2－二取代二茂铁类分子的螺旋结构的来源,指明其结构与旋光方向的关系,然后详细地分析了几个有代表性的1,2－二取代二茂铁类分子的螺旋结构与旋光方向,结果表明：二价铁离子与两个取代基的相互作用力以及两个取代基之间的相互作用力共同决定着指定构型的二茂铁会形成哪种螺旋,从而呈现一定的旋光方向。     

对3种不同硫化物自组膜免疫传感器的比较研究

在半胱氨酸自组膜上固定抗体（羊抗小鼠IgG）制备免疫传感器,分别与巯基十一酸自组膜和32-巯基-3,6,9,12,15,18,21-七氧杂三十二烷酸（EG6COOH）自组膜免疫传感器比较其性能。结果发现通过半胱氨酸自组膜制备的免疫传感器具有最好的灵敏度。能够在13min内。0．05～5．4μg／L范围对游离IgG灵敏检测,检测下限为0．05μg／L。     

协同讨论观点影响度分析及其可视化实现

随着大量网络协同讨论平台的产生,讨论的参与者已经突破了地域的限制,讨论的内容与深度也随之爆炸性地增长。在含有大量冗余信息的讨论中,快速找到讨论的核心与当前热点话题,是推进讨论快速进行的关键。文章提出一种观点影响度分析方法,通过基于Hownet语义词典的语义相似度分析方法,帮助讨论观点自动分类,并通过可视化手段将观点之间的影响程度实时展现出来,辅助人们在杂乱的讨论过程中把握中心观点和当前热点。     

Effect of density of hydrogen-bonding donor on hydrogen-bonded multilayer buildup

The effect of density of hydrogen-bonding donor （HBD） on the formation of layer-by-layer assemblies of poly（4-vinylpyridine） and poly（4-vinylphenol） was investigated. For this purpose, a series of ethyl-substituted poly（4-vinylphenol） （EsPVPhf） with variable ethyl substitute percentage was synthesized by grafting the phenol moiety along the poly（4-vinylphenol） backbone with 1-bromoethane. UV-vis spectroscopy revealed a uniform deposition process of the hydrogen-bonded multilayer consisting of poly（4- vinylpyridine） （PVPy） and EsPVPhf with variable density of HBD. Notably, it was found that increasing the HBD density of EsPVPhf resulted in a marked decrease of both amount of polymers adsorbed and film thickness, which should be related to the EsPVPhf conformation change from coiled state to extended conformation in ethanol solution. Compared with the effect of charge density in polyelectrolyte multUayer, however, there does not exist a critical density of HBD in our case of hydrogen-bonded multilayer assembly. In addition, surface structures of PVPy/EsPVPhf multilayer films also can be tailored controllably by adjusting HBD density of EsPVPhf. As a result, a new method for tuning the structure of hydrogen-bonding-directed multilayer films was developed.