基于DNA折纸模板的铁原子阵列构建及其信息加密应用

在后摩尔时代,突破原有技术极限,进行原子尺度的精准构筑,是当前的重大科学问题.DNA作为具有原子级精准度的生物大分子,能够进行程序性的分子识别,构筑原子数量与位置均严格确定的自组装结构,因此是进行原子制造的理想平台.本文提出基于DNA自组装折纸结构的精准定位能力,构筑铁原子阵列图案,并应用于对信息的加密.实验结果表明,采用类似“信息预置”的方法,铁原子成功实现在DNA折纸不同位置的高效定位,此方法还极大降低了实验工作量,非常有利于多种不同阵列图案的平行制备.利用所构建的铁原子阵列,本文发展了原子阵列DNA折纸加密技术,将密文编码为二进制并用类似盲文斑点的形式在DNA折纸上以特定图案表示,通过单分子成像手段对密文信息进行了读取,而密钥长度可高达700位以上.作为示例,成功地对普通文本及唐诗《登鹳雀楼》进行了加密,证明了此策略的通用性和实用性.     

石墨烯纳米结构的原子级精准构造

相比单层石墨烯,特定构型的石墨烯纳米结构具有更加新奇的物理性质,被认为是构筑基于石墨烯功能纳米器件的基本单元。由于纳米结构的性质对其局域原子构型非常敏感,可控制备高质量的、原子级精确的石墨烯纳米结构并研究其奇特的电子学和自旋电子学性质是实现其器件应用的必要前提。目前,实验构筑锯齿形石墨烯纳米带及其面内异质结、纳米孔洞以及量子点已取得很多重要进展,但是具有复杂结构的功能化石墨烯纳米结构的构筑与物性研究仍存在挑战。文章介绍作者在原子级精确构造石墨烯纳米结构方面取得的系列科研进展。运用可控制备技术与高精度的极低温强磁场扫描隧道显微镜,探索在不同衬底上制备高质量的、具有特定构型的石墨烯纳米结构,并尝试对制备的石墨烯纳米结构进行原子级精准的操纵,实现构造"用户定制"的功能化石墨烯纳米结构。此系列工作发展了石墨烯纳米结构精确可控制备方法,为研究复杂纳米结构与物性提供了新的思路。     

基于原子操纵技术的人工量子结构研究

扫描隧道显微镜原子操纵技术是指利用扫描探针在特定材料表面以晶格为步长搬运单个原子或分子的技术.它是纳米尺度量子物理与器件研究领域一种独特而有力的研究手段.利用这种手段,人们能够以原子或分子为单元构筑某些常规生长或微加工方法难以制备的人工量子结构,通过对格点原子、晶格尺寸、对称性、周期性的高度控制,实现对局域电子态、自旋序、以及能带拓扑特性等量子效应的设计与调控.原子操纵技术与超快测量及自动控制技术的结合,使得人们能够进一步研究原子级精准的量子器件,因而该技术成为探索未来器件新机理、新工艺的重要工具.本文首先简介原子操纵方法的发展过程和技术要点,然后分别介绍人工电子晶格、半导体表面人工量子点、磁性人工量子结构、人工结构中的信息存储与逻辑运算、单原子精度原型器件等方面的最新研究进展,以及单原子刻蚀和自动原子操纵等方面的技术进展,最后总结并展望原子操纵技术的应用前景和发展趋势.     

核酸-金属复合物及其在原子制造领域的应用

原子及近原子尺度制造是直接以原子为操纵对象,构建具有特定功能的原子尺度结构,并实现批量生产以满足所需要的前沿制造技术,是国际学术研究的前沿热点问题.本综述总结了核酸材料在精准原子制造中的应用及前景,从核酸材料的基本结构与功能出发,论述了DNA与金属原子相互作用的基本原理.从天然核酸材料、人工碱基"分子元素"、核酸纳米结构等方面分类介绍了核酸材料介导的精准原子制造的发展历程与突破性进展.最后,对该领域存在的一些挑战与机遇进行了系统性总结,并对其未来发展方向进行了展望.     

从“纳米原子”到“巨型分子”的软物质研究

本文通过分析软物质科学发展的趋势,回顾了"纳米原子"与"巨型分子"这类新型软物质材料的发展历程,总结了"纳米原子"的结构特点以及"巨型分子"自组装的若干特色,提出将"纳米原子"作为"巨型分子"的基本"结构子"和"功能子",以实现模块化的精确结构高分子理性设计与精准合成,并进一步实现其可控组装,调节其多级结构(特别是1—100 nm尺度的结构),最终实现其多样的功能化.这种具有高度刚性构型和固定形状尺寸的大分子有别于传统大分子的柔性链式结构,在组装中也呈现出了与传统大分子截然不同的有趣相态和相结构,是大分子科学的一类新元素,值得进行深入研究.     

功能纳米结构的组装和物性调控

功能纳米结构的组装与物性调控是纳米电子器件前沿基础研究领域的重要问题.本文对我们实验室在纳米自组装结构和物性调控方面的主要研究进展进行介绍.对扫描隧道显微镜(STM)的成像机制和针尖功能化问题进行了研究和探讨.选用不同的策略和方法来实现功能分子在金属单晶基底上的可控自组装,形成各种自组装有序结构,通过磁性分子吸附构型的改变来实现对金属表面上单分子自旋态的量子调控.     

表面原子操纵与物性调控研究进展

利用扫描隧道显微镜可以在单原子层次上对材料进行操纵,改变其结构与特性,实现原子级结构与物性的精准调控.近年来,扫描隧道显微镜原子操纵技术被广泛用于新型低维材料的精准构筑与物性调控.本文主要介绍应用原子操纵技术对低维材料物性调控的最新研究进展,总结了4种主要探针操纵模式:1)探针局域电场模式; 2)调节探针-样品垂直间距模式; 3)无损形态调控模式; 4)可控裁剪刻蚀模式.通过这些探针操纵模式引入局域的电场、磁场、应力场等,实现在单原子层次上对低维材料的电荷密度波、近藤效应、非弹性隧穿效应、马约拉纳束缚态等新奇物性进行精准地调控.     

气相沉积技术在原子制造领域的发展与应用

随着未来信息器件朝着更小尺寸、更低功耗和更高性能方向的发展,构建器件的材料尺寸将进一步缩小.传统的"自上而下"技术在信息器件发展到纳米量级时遇到瓶颈,而气相沉积技术由于其能在原子尺度构筑纳米结构引起极大关注,被认为是最有潜力突破现有制造极限进而在原子尺度构造、搭建物质形态的"自下而上"方法.本文重点讨论适用于低维材料的原子尺度制造的分子束外延技术和原子层沉积/刻蚀技术.简要介绍相关技术中蕴含的科学原理及其在纳米信息器件加工和制造领域的应用,并探讨如何在原子尺度实现对低维功能材料厚度和微观形貌的精密控制.     

功能分子结构的组装和单分子物性：基于密度泛函理论的第一性原理计算与扫描隧道显微学（Ⅰ）

在单个分子的层次上研究低维分子纳米结构的生长,理解组装机制并实现结构与特性的有效控制,是低维体系物理及其器件研究的重要内容.本文在基于密度泛函的第一性原理计算的基础上,对功能分子在金属表而上的自组装特性等进行了综述.对理论方法作了简要介绍后,综述了第一性原理计算方法在研究金属基底上分子自组装结构、界面特性、结构控制、单分了成像机制、单分子量子调控以及单分子输运性能等方面的应用.最后对基于密度泛函的第一性原理计算在解释功能分子组装与界面物理化学特性方面的发展前景进行了展望.     

{（Eu（PW11）2）m/PEI}多层纳米复合膜的制备和光谱表征

在科技竞争日益激烈的今天,功能性分子材料的设计和获得是科学界面临的主要挑战之一.多金属氧酸盐因其具有特定的结构和优越的光、电和磁等物理化学性质,已经成为构造新型功能材料的重要无机构筑块.借助于分子间弱的相互作用将多金属氧酸盐引入到纳米复合薄膜材料中,利用无机和有机组分的协同作用来诱导和产生新的功能特性,必定会给这种无机构筑块在材料科学中的应用创造更多的机会.静电沉积技术是制备有机一无机超薄膜的一种有效方法,人们已经成功地实现了各种无机材料的组装,它们在非线形光学、导电膜、电致发光器件和传感器等方面有着潜在的应用前景.利用层层自组装法(layer bylayer self assembly,LBL),制备出有序且稳定的多金属氧酸盐Eu(PW111)2的多层膜.应用紫外光谱研究其层层组装过程,观察到层层组装是一个均一过程.荧光光谱研究表明所制备的含稀土多金属氧酸盐阴离子的多层膜,通过调节膜的厚度、组成和结构,多层膜具有Eu3 的特征发射.这一结果为发光器件的发展提供了丰富的数据.     

Self‐Assembly of Ag6 Clusters into Nanowires for Nonenzymatic Electrochemical Sensing of Glucose

Self‐assembly of metal nanoclusters into 3D ordered superstructures and the exploration of their electrochemical properties are highly significant for fundamental research and practical application. In this study, atomically precise Ag₆(NALC)₅ nanoclusters are successfully synthesized and their structure is determined carefully. It is interesting that the prepared Ag₆(NALC)₅ nanoclusters can be self‐assembled into ultrafine nanowires, long ribbons, and finally 3D porous network in the mixed solution of water and ethanol, which can be attributed to the solvent polarity, static electricity interaction between ligands, and the possible Van der Waals attractions. Such assembly phenomenon lays a foundation for the future fabrication of silver clusters‐based nanodevices. In addition, the synthesized silver nanoclusters can be used for electrochemical sensing of glucose with high detection sensitivity, selectivity, and low limit of detection. This work is expected to be helpful for the synthesis of atomically precise metal nanoclusters and their applications in fabrication of nanodevices for chemical sensors.     

Magnetic Coupling Induced Self-Assembly at Atomic Level

Developing accurate self-assembly is the key for constructing functional materials from a bottom-up approach.At present, it is mainly hindered by building blocks and driving modes. We design a new self-assembly method based on the magnetic coupling between spin-polarized electrons. First-principles calculations show that spinpolarized electrons from different endohedral metallofullerene(EMF) superatoms can pair each other to ensure a one-dimensional extending morphology. Furthermore, without ligand passivation, the EMF superatoms maintain their electronic structures robustly in self-assembly owing to the core-shell structure and the atomic-like electron arrangement rule. Therefore, it should noted that the magnetic coupling of monomeric electron spin polarization can be an important driving mechanism for high-precision self-assembly. These results represent a new paradigm for self-assembly and offer fresh opportunities for functional material construction at the atomic level.     

Site equivalent all Apex 1 nm-particle of CdSe preferentially grown in solution

A 1-nm particle of CdSe showing a sharp photoabsorption peak at 350 nm has been selectively synthesized as a single species in solution. Solid NMR spectra of both atoms show a single narrow peak of large chemical shift anisotropy and asymmetry compared with the essentially isotropic bulk CdSe. This result indicates that this extremely small 1-nm particle has most of its atoms at the surface, and the atoms are deformed from the sp³ configuration of the bulk fragment into an assembly consisting entirely of apexes of equivalent symmetry that are particularly stable and preferentially grown. This observed selective stability presents the possibility of growing 1-nm particles with an atomic monostructure in macroscopic quantities.     

Atomic spectroscopy and quantum optics in hollow‐core waveguides

Atomic spectroscopy is a well‐established, integral part of the physicist's toolbox with an extremely broad range of applications ranging from astronomy to single atom quantum optics. While highly desirable, miniaturization of atomic spectroscopy techniques on the chip scale was hampered by the apparent incompatibility of conventional solid‐state integrated optics and gaseous media. Here, the state of the art of atomic spectroscopy in hollow‐core optical waveguides is reviewed The two main approaches to confining light in low index atomic vapors are described: hollow‐core photonic crystal fiber (HC‐PCF) and planar antiresonant reflecting optical waveguides (ARROWs). Waveguide design, fabrication, and characterization are reviewed along with the current performance as compact atomic spectroscopy devices. The article specifically focuses on the realization of quantum interference effects in alkali atoms which may enable radically new optical devices based on low‐level nonlinear interactions on the single photon level for frequency standards and quantum communication systems.     

Semiconductor nanowires for novel one-dimensional devices

Low-dimensional semiconductors offer interesting physical phenomena but also the possibility to realize novel types of devices based on, for instance, 1D structures. By using traditional top-down fabrication methods the performance of devices is often limited by the quality of the processed device structures. In many cases damage makes ultra-small devices unusable. In this work we present a recently developed method for bottom-up fabrication of epitaxially nucleated semiconductor nanowires based on metallic nanoparticle-induced formation of self-assembled nanowires. Further development of the vapor–liquid–solid growth method have made it possible to control not only the dimension and position of nanowires but also to control heterostructures formed inside the nanowires. Based on these techniques we have realized a series of transport devices such as resonant tunneling and single-electron transistors but also optically active single quantum dots positioned inside nanowires displaying sharp emission characteristics due to excitons.     

解读生命密码——人类基因组计划

DNA测序技术的自动化使得人类基因组测序工作在启动10年后就已接近完成,从物理学的角度来,生物体是工作在单分子水平上的多层次综合的信息、能量和物质加工转换系统,关于生物生长发育和遗传的信息记录在线型分子——核酸的碱基序列中,每个基因是编码一个蛋白质的核酸片段,这些蛋白质分子是机器的主要零部件,首次人类基因组测序的完成,只是生命密码破译的开始,而不是结束,年轻的物理学家应积极地参与揭示生命本质的活动。     

Highly Efficient Fabricating Amorphous Photonic Crystals Using Less Polar Solvents and the Wettability-Based Information Storage and Recognition

Facile and efficient fabrication of amorphous photonic crystals (APCs) with uniform and angle independent structural colors is highly desired due to their unique applications in non-iridescent colors-based displays, pigments, and sensors. Here, a solvent-assisted colloidal assembly approach is reported to fabricate APCs with uniform and angle-independent structural colors by the self-assembly of polydopamine-embedded silica particles in pentanol. The surface charge of the particle mediated by the polarity of solvent is demonstrated to be the key to control the particle arrangements and the angle dependency of the structural colors, which makes the fabrication more efficient, simple, and convenient compared to previous methods. Owing to the amorphous structures, the APCs show unique sensitivity to the variation of the refractive index contrast. Based on this unique sensitivity of APCs, an information storage-recognition system is established by constructing different wettability between the information and background region. The information integrated with the color, the number, and the site of APCs of the system can be stored and recognized at dry and wetting state, respectively, and the switching of the storage-recognition process is fully reversible. These findings provide new insights into the design, fabrication, and application of materials with non-iridescent structural colors.