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框架核酸是核酸分子通过自组装形成的一维到三维的框架结构, 不仅能精准定位功能基元, 还可实现在纳米甚至原子级尺度上进行力学、光学和电学等物理性质, 以及单分子水平化学与生化反应的精准调控. 利用框架核酸对物质进行原子级的人工自组装, 可实现基本构筑单元的精准物理排布与功能化集成, 进而实现器件制造, 有望推动从原子到宏观的精确功能化的制备. 本文围绕框架核酸和原子制造两大前沿的交叉领域, 阐述框架核酸在原子级精准构筑方面的可行性和优势, 首先介绍了具有原子级精准性的框架核酸的构建, 以及利用框架核酸进行功能化组装的一般策略, 然后着重探讨框架核酸在器件构筑方面的研究进展, 最后就面向原子制造的未来发展方向进行了展望.In recent years, the technology of traditional integrated circuit fabrication is facing a huge challenge. As the top-down lithography gradually approaches to its size limit, the development of atomic-scale precise fabrication for functional devices has already become a major scientific issue at present and might become a breakthrough in the development of information technology in the future. With the reference of the bottom-up self-assembly, which is the basic principle of constructing various advanced structures in living systems, the integrated assembly of atoms can be gradually constructed through a series of operations such as capturing, positioning, and moving atoms. The advent of framework nucleic acids (FNAs) happens to provide a new platform for manipulating single atom or integrating multiple atoms. As is well known, the nucleic acids are not only the carriers of genetic information, but also biological building blocks for constructing novel microscopic and macroscopic materials. The FNAs represent a new type of framework with special properties and features, constructed by nucleic acids’ bottom-up self-assembly. With the improvement of chemical synthesis and modification method of nucleic acids, various molecules and materials, such as fluorophores, nanoparticles, proteins, and lipids, can be spatially organized on FNAs with atomic precision, and these functionalized FNAs have been widely explored in the fields of biosensing, biocomputing, nano-imaging, information storage, nanodevices, etc. Based on the features of precise addressability, superior programmability and tailorable functionality, FNAs can be used for implementing the artificial self-assembly of objects with atomic precision to realize the precise arrangement in spatial and functional integration of basic assembly units, and even prompt the development of device fabrication from atomic scale to macroscopic scale. This review focuses on the intersection of FNAs and atomic fabrication, giving a systematically description of the feasibility and advantages of precisely atomic fabrication with FNAs from three aspects. First, the DNA/RNA nanoarchitectures from static state to dynamic state and general strategies for programmable functionalization of FNAs are briefly introduced. Then the applications of FNAs in device fabrication are highlighted, including single molecule reactors, single molecule sensors, nanodevices for cargo loading and transporting, nanophotonics, nanoelectronics and information processing devices. Finally, an outlook of the future development of atomic fabrication with FNAs is given as well.
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Keywords:
- framework nucleic acids /
- atomic fabrications /
- self-assembly /
- functional devices
1. 引 言
尘埃等离子体由电子、离子、中性粒子和尘埃颗粒组成, 在空间物理[1,2]、半导体工业领域[3]、聚变[4]以及实验室[5-9] 中受到广泛研究. 尘埃颗粒与等离子体中的电子和离子频繁碰撞而携带电荷, 通过颗粒间的相互作用形成强耦合系统. 在实验室研究中, 这一特性使尘埃等离子体成为模拟许多微观物理过程的理想平台, 如结晶[10-12]、相变[13-15]、孤波[16,17]和马赫锥[18,19]等. 尘埃颗粒通过粒子-粒子以及粒子-波等相互作用形式从等离子体中获取能量, 这些尘埃颗粒的动能可以高达上百个eV[20,21]. 然而, 通常情况下尘埃颗粒悬浮在极板鞘层附近进行随机运动, 其携带的能量不能被有效地收集并利用. 因此, 如何将尘埃颗粒的随机运动整流成定向运动成为解决这一问题的关键.
费曼棘轮可以将粒子的随机运动转化为定向运动, 且不违反热力学第二定律[22,23]. 费曼棘轮通常由具有一定不对称性的周期性棘轮单元组成, 由于费曼棘轮原理的普适性与重要性, 关于它的研究已经延伸到量子棘轮[24,25]、有机电子棘轮[26]以及光学棘轮[27]等学科领域. 这些系统中具有的某种对称性破缺机制是费曼棘轮运行的关键. 这些棘轮实验主要集中在微纳尺度的棘轮结构、超导下或者液相环境下, 实现条件普遍比较苛刻且实验难度较大. 近期, 研究者们利用尘埃等离子体系统易于实验和便于观察等特点, 将费曼棘轮原理引入到尘埃等离子体物理领域, 设计出尘埃等离子体圆棘轮, 实现了对尘埃颗粒的可控性整流, 即将尘埃颗粒的随机运动整流为定向运动[28]. 系统中的不对称性来源于水平极板上两个圆形树脂棘轮围成的棘轮通道, 带电尘埃颗粒在棘轮通道中受到棘轮势的作用, 形成的棘轮效应使得尘埃颗粒可以沿棘轮通道定向输运. 由于树脂棘轮位于极板上的鞘层内, 其形成的是悬浮电位, 在实验中很难精确控制其电位进而有效调控棘轮势与颗粒输运. 如果使用金属棘轮并将其置于极板上, 金属棘轮可以与极板同电位, 通过调节放电条件可准确控制金属棘轮电位, 并且可使其具有更低的电位水平, 由此可实现对棘轮势在较大范围内的精确调控, 此时, 尘埃颗粒输运可能会有新现象, 这方面的实验研究还未见报道. 本文通过设计尘埃等离子体金属直棘轮实验装置, 研究了微米级单分散尘埃颗粒在不同放电条件下的整流规律以及不同尺寸尘埃颗粒在相同放电条件下的整流现象, 进一步通过等离子体流体模拟获得等离子体参量的二维分布, 并基于Langevin方程对不同尺寸颗粒的运动进行数值模拟, 在相同条件下分析不同尺寸的尘埃颗粒在尘埃等离子体金属直棘轮中的整流机制.
2. 实验装置
图1为尘埃等离子体金属直棘轮实验装置示意图. 在尺寸为30 cm×20 cm×15 cm的真空室内水平放置两个极板, 上极板氧化铟锡(ITO)玻璃接地, 下极板不锈钢板接13.56 MHz的射频电源和匹配器. 下极板的上表面由30个宽为5 mm和高为3 mm的锯齿槽构成(如图1所示依次编号), 其沿x方向具有不对称性和周期性变化特点. 同时, 在下极板上面沿x方向平行设置两个金属条, 其下表面具有与下极板相同尺寸的锯齿槽, 并与下极板完全啮合. 两金属条之间距离为10 mm, 因此, 两个金属条和下极板构成沿x方向的棘轮通道. 利用容性耦合氩气辉光放电产生均匀的等离子体后, 棘轮通道表面形成鞘层, 其沿x方向具有不对称性与周期性分布特征. 利用颗粒注射器在棘轮通道中间“0”号锯齿槽处持续不断地缓慢投入微米大小的聚苯乙烯微球(尘埃颗粒). 这些尘埃颗粒在等离子体中自由下落时快速充电, 在受到下极板鞘层电场的作用下一般悬浮于棘轮通道上方4—8 mm处, 在一定的实验条件下能够沿棘轮通道形成定向输运, 当棘轮通道内所有锯齿槽均被尘埃颗粒填满时, 尘埃颗粒会流出棘轮通道并流入棘轮通道两端外侧的收集槽中. 通过调节放电条件或使用不同大小的尘埃颗粒, 可以控制尘埃颗粒的输运方向与速度. 为了方便观测, 在真空室外两侧相向沿棘轮通道方向施加两束5 mW的激光束(532 nm)用于照明尘埃颗粒, 尘埃颗粒的运动状态利用位于真空室上方的摄像机进行记录. 为了研究金属直棘轮中尘埃颗粒的整流机制, 分别使用直径为10, 15和 24 µm的单分散聚苯乙烯微球进行实验, 气压p变化范围是20—50 Pa, 功率P变化范围是10—50 W.
图 1 尘埃等离子体金属直棘轮实验示意图. 下极板的上表面由30个锯齿槽构成(图中只显示7个), 结合两个金属条, 形成沿x方向的棘轮通道. 单分散尘埃颗粒由棘轮通道中部的“0”号锯齿槽投入, 在特定条件沿棘轮通道会产生定向运动Fig. 1. Schematic diagram of the dusty plasma metal straight ratchet. The upper surface of the lower electrode is composed of 30 sawteeth (shown only 7 sawteeth), combined with two metal strips, a ratchet channel along the x direction is formed. Monodispersed dust particles are introduced into the “0” sawtooth at the middle of the ratchet channel, which exhibit directional flow along the ratchet channel under specific conditions.3. 实验结果
利用尘埃等离子体金属直棘轮能够实现尘埃颗粒的整流. 为了展示整流现象, 实验中从棘轮通道中间“0”号锯齿槽处持续地撒入直径为15 µm的单分散尘埃颗粒, 并观察尘埃颗粒的运动情况. 尘埃颗粒在等离子体中自由下落时快速充电, 在落入棘轮通道后受下极板及两侧金属条鞘层电场作用悬浮并被约束在棘轮通道的中间位置. 当单个锯齿槽中只有少量尘埃颗粒时, 尘埃颗粒在锯齿槽中呈现单链分布, 如果继续加入尘埃颗粒, 由于颗粒间Yukawa静电排斥作用, 尘埃颗粒在单个锯齿槽内形成中间双链两端单链的分布, 此时单个锯齿槽中的尘埃颗粒达到饱和, 约有nmax=17个, 此过程如图2(a), (c)和(e)中局部放大插图所示. 这个饱和颗粒数nmax的大小与尘埃颗粒半径和放电条件有一定的关系, 但是影响不大, 只有2—3个的差别. 此时, 再继续加入尘埃颗粒, 在颗粒间相互作用力和带电颗粒之间的集体效应的推动下, 尘埃颗粒分布由“0”号锯齿槽向其相邻的锯齿槽扩展, 如图2(a), (b)所示, 此时尘埃颗粒并没有形成持续的单方向输运(整流). 如果持续不断地撒入尘埃颗粒, 棘轮的整流效应开始显现出来, 在非平衡离子拖拽力的作用下[28], 尘埃颗粒由“0”号锯齿槽依次流入“1”, “2”, “3”, ⋯号锯齿槽进而形成持续的正向输运, 即正流, 如图2(c)—(f)所示. 特别要注意的是, “–1”号锯齿槽在初始撒颗粒时会涌入少量颗粒, 在尘埃颗粒形成持续的整流后, “–1”号锯齿槽内颗粒数逐渐饱和, 其左侧的“–2”号等锯齿槽内的颗粒数为 0, 如图2(e)所示. 图2(b), (d), (f)分别给出了随着颗粒数的增加颗粒数N在棘轮通道内的分布与演化过程. 此外, 当停止向棘轮通道中撒入尘埃颗粒时, 棘轮通道内的尘埃颗粒将在各自的平衡位置上趋于静止, 这是由于尘埃颗粒的动能小于沿棘轮通道x方向的棘轮势能, 尘埃颗粒被束缚在棘轮势阱中, 此时尘埃颗粒不能形成沿棘轮通道持续的输运, 只有持续不断地向棘轮通道中撒入尘埃颗粒时, 棘轮通道内尘埃颗粒的平衡状态才会被打破, 尘埃颗粒才会沿着棘轮通道形成持续的正流. 尘埃颗粒的定向输运速度与往“0”号锯齿槽中投入颗粒数的速率有关, 在本次实验中, 尘埃颗粒形成稳定正流后的平均速度约为0.53 mm/s. 因此, 当放电气压p=35 Pa, 放电功率P=40 W时, 尘埃等离子体金属直棘轮中颗粒形成正流.
图 2 尘埃等离子体金属直棘轮中尘埃颗粒的正流 (a), (c), (e)随着投入尘埃颗粒数的增加, 尘埃颗粒在棘轮通道中的空间分布逐渐向右扩展, 形成正向整流, 图中N代表棘轮通道中尘埃颗粒总数量; (b), (d), (f)对应的不同锯齿槽位置处颗粒数n的分布情况, 放电气压为 , 放电功率为p=35 Pa , 颗粒直径为15 µm. 图中尘埃颗粒做了亮度增强处理P=40 W Fig. 2. Positive flow of dust particles in the dusty plasma metal straight ratchet: (a), (c), (e) Number of introduced dust particles increases, the spatial distribution of dust particles in the ratchet channel gradually expands to the right, forming a positive flow, N represents the total number of dust particles in the ratchet channel; (b), (d), (f) the corresponding distributions of particle number n along the ratchet channel, gas pressure , discharge powerp=35 Pa , particle diameter is 15 µm. Brightness of dust particles in images is enhanced.P=40 W 通过改变放电功率可以改变尘埃颗粒的整流速度. 当保持放电气压p=35 Pa不变, 逐渐降低放电功率会导致尘埃颗粒整流速度的减缓, 当放电功率降至P=25 W时, 尘埃颗粒将无法形成定向输运. 在新的一次实验中(P=25 W), 从棘轮通道中间“0”号锯齿槽处缓慢地撒入尘埃颗粒. 刚开始时, 由于撒入的颗粒数量较少且受到棘轮电势的约束, 尘埃颗粒会积聚在“0”号锯齿槽内. 随着撒入颗粒数N的增加, 由于带电尘埃颗粒之间的排斥作用, “0”号锯齿槽不能再容纳下这些尘埃颗粒, 它们将在集体效应的作用下以近似相等的速度均匀地向“0”号锯齿槽两侧流动, 直到这些尘埃颗粒均匀分布并铺满整个棘轮通道, 如图3(a), (c), (e)所示. 从图3(b), (d), (f)所示的尘埃颗粒在棘轮通道中的分布曲线可以看出, 随着尘埃颗粒数量的增加, 颗粒的分布曲线逐渐向棘轮通道两端同时上扬, 并且在“0”号锯齿槽(虚线位置)附近呈现出明显的对称性, 这表明尘埃颗粒沿棘轮通道输运的净位移为零. 此时, 尽管尘埃颗粒表现出双向输运现象, 但这一现象并非源自棘轮势的影响, 而只是由颗粒之间的相互排斥作用引起的.
图 3 尘埃等离子体金属直棘轮中尘埃颗粒的无净位移运动 (a), (c), (e)随着投入尘埃颗粒数的增加, 尘埃颗粒在棘轮通道中的空间分布逐渐向两侧同时扩展, 图中N代表棘轮通道中尘埃颗粒总数量; (b), (d), (f)对应的不同锯齿槽位置处颗粒数n的分布情况. 放电气压为 , 放电功率为p=35 Pa , 颗粒直径为15 µm, 图中尘埃颗粒进行亮度增强处理P=25 W Fig. 3. None net flow of dust particles in the dusty plasma metal straight ratchet: (a), (c), (e) Number of introduced dust particles increases, the spatial distribution of dust particles in the ratchet channel gradually expands to both sides simultaneously, N represents the total number of dust particles in the ratchet channel; (b), (d), (f) the corresponding distributions of the particle number n along the ratchet channel, gas pressure , discharge powerp=35 Pa , particle diameter is 15 µm, brightness of dust particles in images is enhanced.P=25 W 通过改变放电功率还可以进一步控制尘埃颗粒的整流方向. 在新的一次实验中, 保持放电气压p = 35 Pa不变, 将放电功率降到P=15 W时, 从棘轮通道中间“0”号锯齿槽处逐渐撒入尘埃颗粒. 随着撒入颗粒数量的增加, 颗粒会从“0”号锯齿槽依次流入“–1”, “–2”, “–3”, ⋯号锯齿槽进而形成持续的逆向输运, 即逆流, 如图4(a), (c)和(e)所示. 在经过约50 s后, 尘埃颗粒在棘轮通道中形成稳定的逆流. 此时棘轮通道中尘埃颗粒的分布不会再随时间的推移而发生显著变化. 在此过程中, 尘埃颗粒的数量分布曲线向棘齿通道左侧逐渐上扬直到饱和, 如图4(b), (d), (f)所示. 此时, 如果停止投入尘埃颗粒, 这种持续的尘埃颗粒整流过程将中断, 这与图2所示的尘埃颗粒正流过程类似. 在本次实验中, 尘埃颗粒沿棘轮通道形成稳定逆流后的平均速度约为–0.12 mm/s. 通过对比图2—图4发现, 在保持放电气压p=35 Pa不变的情况下, 随着放电功率的逐渐降低, 尘埃颗粒沿棘轮通道的整流速度表现出由正向逐渐降低至零并进一步转为逆向, 发生了流的反转现象.
图 4 尘埃等离子体金属直棘轮中尘埃颗粒的逆向整流 (a), (c), (e)随着投入尘埃颗粒数的增加, 尘埃颗粒在棘轮通道中的空间分布逐渐向左扩展, 形成逆向整流. 图中N代表棘轮通道中尘埃颗粒总数量. (b), (d), (f)对应的不同锯齿槽位置处颗粒数n的分布情况. 放电气压为 , 放电功率为p=35 Pa , 颗粒直径为15 µm. 图中尘埃颗粒做了亮度增强处理P=15 W Fig. 4. Negative flow of dust particles in the dusty plasma metal straight ratchet: (a), (c), (e) Number of introduced dust particles increases, the spatial distribution of dust particles in the ratchet channel gradually expands to the left, forming a negative flow, N represents the total number of dust particles in the ratchet channel; (b), (d), (f) the corresponding distributions of the particle number n along the ratchet channel. Gas pressure , discharge powerp=35 Pa , particle diameter is 15 µm. Brightness of dust particles in images is enhanced.P=15 W 尘埃颗粒整流及其反转的现象不仅与放电功率的变化有关, 还与放电气压密切相关. 通过对放电气压和放电功率进行较大范围的参数扫描, 将其对尘埃颗粒整流行为的影响绘制成相图, 如图5所示. 在该相图中, 黑色曲线为尘埃颗粒呈现正、逆流的临界线, 即在这条黑色临界线上对应的放电功率与气压条件下尘埃颗粒沿棘轮通道的净位移为零(没有定向输运), 在临界线上方区域的实验条件下尘埃颗粒形成正流, 反之形成逆流. 这表明, 尘埃颗粒的整流可以在一个较为宽泛的放电功率和气压条件下实现, 并且, 在较高气压和较高放电功率的条件下尘埃颗粒更容易发生正流现象, 而在较低气压和较低放电功率的条件下尘埃颗粒则更容易发生逆流现象. 因此, 图5表明, 通过调节放电功率和气压能够精确调控尘埃颗粒的整流方向. 此外, 尘埃颗粒的投入速度对尘埃颗粒整流速度的大小有一定的影响, 由于实验中很难实现匀速定量的投入尘埃颗粒, 导致尘埃颗粒的整流速度不太稳定, 所以目前很难在相图中同时给出整流速度大小与放电功率和气压的关系.
图 5 不同放电气压和功率实验条件下尘埃颗粒整流的相图. 黑色曲线表示尘埃颗粒在棘轮通道中呈现正流和逆流的临界线, 颗粒直径为15 µmFig. 5. Phase diagram of the directional flow of dust particles under different gas pressure and power experimental conditions. The black curve represents the critical line separating the positive and negative flows of dust particles in the ratchet channel, particle diameter is 15 µm.以上实验结果展示了直径为15 µm的单分散尘埃颗粒在不同放电条件下的整流现象. 由于尘埃颗粒在棘轮通道中的悬浮高度与其直径密切相关, 因此, 不同直径的尘埃颗粒的悬浮高度不同, 所处的等离子体环境不同, 进而其整流行为也不相同. 通过对不同直径(10, 15和24 µm)的尘埃颗粒在相同装置中的整流行为进行系统研究, 结果表明这些尺寸的尘埃颗粒在棘轮通道中均可实现整流, 但其正流和逆流发生转变的临界放电条件存在一定差异, 这些差异并不影响尘埃颗粒定向输运的定性结论. 图6给出了在放电气压p=35 Pa, 放电功率P=25 W的实验条件下, 这3种尺寸尘埃颗粒在棘轮通道中的整流情况. 实验结果表明, 在这一放电条件下, 直径为10 µm和24 µm的尘埃颗粒在棘轮通道中分别形成正流(平均速度约0.39 mm/s)和逆流(平均速度约–0.11 mm/s), 分别如图6(a), (c)所示, 而直径为15 µm的尘埃颗粒在棘轮通道中没有形成定向输运(净位移为零, 图6(b)). 通过测量进一步发现, 随着尘埃颗粒直径的增大, 其在棘轮通道中的悬浮高度分别由z = 5.9 mm降低到4.7 mm和4.1 mm, 因此, 尘埃颗粒的悬浮高度影响了其输运结果. 此外, 在图5所示相图的放电参数范围内, 直径在 5—35 µm范围内的尘埃颗粒都可以进行整流.
图 6 同一放电条件下不同尺寸尘埃颗粒在棘轮通道内的运动情况 (a)直径为10 µm的尘埃颗粒随着投入颗粒数目的增加逐渐形成正流; (b)直径为15 µm的尘埃颗粒在棘轮通道中没有形成定向输运; (c)直径为24 µm的尘埃颗粒随着撒入颗粒数目的增加逐渐形成逆流, 放电气压 , 功率p=35 Pa . 图中尘埃颗粒做了亮度增强处理P=25 W Fig. 6. The flow of dust particles with different sizes in the ratchet channel under same discharge conditions: (a) Dust particles with a diameter of 10 µm gradually form a positive flow as the number of introduced dust particles increases; (b) dust particles with a diameter of 15 µm do not form a directional flow in the ratchet channel; (c) dust particles with a diameter of 24 µm gradually form a negative flow as the number of introduced particles increases, gas pressure , discharge powerp=35 Pa . Brightness of dust particles in images is enhanced.P=25 W 4. 数值模拟
尘埃颗粒在棘轮通道中的定向输运与其周围的鞘层等离子体参量密切相关. 为了揭示金属直棘轮中尘埃颗粒整流机制, 首先要掌握等离子体参量的分布情况. 由于棘轮通道的空间尺度非常小, 常用的朗缪尔探针不能准确测量此种情况下的电子密度等参量. 因此, 本文基于尘埃等离子体棘轮模型[29,30]通过数值模拟的方法来获得棘轮通道内的等离子体参量. 这里给出主要的模型计算流程.
由于实验中不同尺寸的尘埃颗粒悬浮在不同高度上(z方向), 并沿棘轮通道x方向进行整流, 因此选择沿棘轮通道中心(y = 0处)的x-z平面进行二维数值模拟. 首先, 利用COMSOL软件建立金属直棘轮射频辉光放电流体模型, 以获得下极板锯齿槽表面鞘层的等离子体参量, 由于金属直棘轮呈现周期性排列结构, 模拟中只选取一个锯齿单元作为模拟区域, 并在x方向上采用周期性边界条件, 放电条件为气压p=35 Pa, 功率P=25 W, 其余各项参数均与实验中保持一致. 随后再利用Matlab软件进一步分析尘埃颗粒在鞘层中的动力学过程. 尘埃颗粒在鞘层中受到的主要作用力包括: 重力 Fg、离子拖拽力Fi、中性粒子阻力Fn、颗粒之间的Yukawa作用力FY、鞘层电场力Fe和涨落力Fη, 其Langevin运动方程为
m¨rk=Fg+Fi+Fn+FY+Fe+Fη,k=1,2,⋯,n, (1) 其中, n为颗粒数, m为颗粒质量, 详细的受力公式参见文献[28, 29]. 根据上述方程, 进一步模拟实验中不同尺寸尘埃颗粒在棘轮通道中的整流过程. 由于尘埃颗粒整流实验中使用的气压较高, 带电颗粒间相互作用势能很强, 处于强耦合状态, 其热运动非常弱, 因此在动力学模拟中将涨落力忽略. 锯齿槽中尘埃颗粒的数量为19个, 沿水平方向上等间隔分布, 初始高度z0 = 7 mm, 初始速度为零. 根据模拟得到的等离子体参量, 利用OML理论[31]可以计算出尘埃颗粒的带电量. 以直径为15 µm的尘埃颗粒为例, 其带电量Q约为−105e, 在棘轮通道中的整流过程中, 其带电量基本保持不变.
下极板锯齿槽表面鞘层中垂直方向电场Ez = –∂U/∂z的等值线表现出明显的不对称性和周期性特征, 如图7(a)所示, 这是由锯齿形电极结构所呈现的不对称与周期性变化决定的. 尘埃颗粒在鞘层中的悬浮高度主要依靠重力、鞘层电场力和竖直z方向上的离子拖拽力Fiz的共同作用, 且满足mg + Fiz=QEz, 其中Fiz约为尘埃颗粒重力的3%, 可以忽略. 由于尘埃颗粒在棘轮通道内水平输运时其带电量Q基本不变, 因此, 尘埃颗粒的悬浮高度由Ez决定, 即同一尺寸的单分散尘埃颗粒将沿其对应的电场等值线悬浮在鞘层中. 对于实验中使用的3种尺寸的尘埃颗粒, 它们分别沿各自对应的Ez等值线悬浮在鞘层中, 其平均悬浮高度分别为5.4, 4.3和3.9 mm, 较小的颗粒悬浮高度较高, 较大的颗粒悬浮高度较低, 如图7(a)所示, 这与实验观测结果一致.
图 7 两个锯齿槽上表面的鞘层电场 的等值线分布(a)以及在这些等值线上对应的电势变化(b). 图(a)中鞘层电场的竖直分量Ez 的等值线呈现不对称性分布, 不同尺寸的尘埃颗粒沿不同的Ez 的等值线悬浮于鞘层中; 图(b)中的电势分布具有棘轮势特征, 因此, 不同尺寸的尘埃颗粒悬浮于鞘层不同的高度, 受到的棘轮势具有不同的特征, 进而使得其形成沿棘轮通道不一样的输运结果. 图中红、绿、蓝球分别表示直径为10, 15和24 µm的尘埃颗粒, 放电气压Ez , 功率p=35 Pa P=25 W Fig. 7. The contour distribution of the sheath electric field on the surface of two sawteeth (a) and the corresponding potential variation along these contour curves (b). (a) The contour curves of the vertical component of the sheath electric fieldEz show asymmetric distributions, dust particles of different sizes are suspended along different contour curves within the sheath; (b) the potential distribution has the characteristic of a ratchet potential. Therefore, dust particles of different sizes are suspended at different heights within the sheath, experiencing ratchet potentials with different characteristics, which leads to distinct transport outcomes along the ratchet channel. The red, green and blue balls in the curves indicate dust particles with diameter of 10, 15 and 24 µm, respectively. Gas pressureEz , discharge powerp=35 Pa .P=25 W 鞘层中这些不同Ez等值线上的电势分布具有其各自的分布特点, 如图7(b)所示. 这些电势线的分布具有一定的不对称性与周期性特征, 是典型的棘轮势, 可通过双正弦函数来反映[22]:
U(x)=ΔU[sin(2πx/L)−14sin(4πx/L)]+U0, (2) 式中, L代表一个锯齿单元的长度, ΔU代表棘轮势振幅, U0代表棘轮势偏置, ΔU和U0分别为
ΔU=(Ul−Uh)/2, (3) U0=(Ul+Uh)/2, (4) 其中, Uh为锯齿尖处的电势, Ul为锯齿槽处的电势. ΔU的符号与大小分别决定了棘轮势的不对称取向与势阱高度.
棘轮势决定了尘埃颗粒在棘轮通道中的输运过程. 这是因为棘轮势产生的电场Ex=−∂U/∂x会引起x方向的离子流, 从而对尘埃颗粒施加非平衡离子拖拽力Fix. 棘轮势的不对称性使非平衡的离子拖拽力在单个棘轮势中的积分fix=∫L0Fixdx可不为零, 其量级约为10−13 N, 足以克服同等量级的中性气体阻力[5,32], 进而推动尘埃颗粒形成定向输运. 棘轮势的不对称性取向决定了尘埃颗粒在棘轮通道中的输运方向. 当尘埃颗粒悬浮在鞘层较高位置时, Ul>Uh, 棘轮势具有正取向(ΔU>0), 尘埃颗粒呈现正流, 如图7(b); 当尘埃颗粒处于较低位置处, Ul<Uh, 棘轮势具有负取向(ΔU<0), 尘埃颗粒呈现逆流; 特别是, 在某一中等高度处, 电势呈水平直线分布(ΔU=0), 不对称性消失, 尘埃颗粒不能形成定向输运(净位移为零). 图7数值计算结果表明, 在相同的放电条件下, 不同尺寸的尘埃颗粒悬浮在鞘层不同高度上, 受到的棘轮势取向不同, 进而形成不同的定向输运, 直径10 µm的尘埃颗粒正流速度平均约0.37 mm/s, 直径24 µm的尘埃颗粒逆流速度平均约–0.13 mm/s, 这与图6实验结果基本一致. 此外, 由于尘埃颗粒在鞘层中的悬浮高度还与放电条件有关, 因此, 还可以通过调节放电气压与功率来控制单分散尘埃颗粒的悬浮高度, 进而控制其输运方向, 即图2—图5所示实验结果.
5. 结 论
本文首先通过设计尘埃等离子体金属直棘轮实验装置, 实现了在较大放电参数范围内对尘埃颗粒的可控性整流. 其次, 在相同的放电条件下对不同尺寸的尘埃颗粒进行整流实验, 观察到较小的尘埃颗粒呈现正流, 较大的尘埃颗粒呈现逆流. 最后, 通过对尘埃等离子体金属直棘轮进行二维数值模拟, 研究不同尺寸尘埃颗粒在相同实验条件下的整流机制. 研究结果表明: 不同尺寸的尘埃颗粒在棘轮通道中的悬浮高度存在差异, 小颗粒悬浮在较高位置, 而大颗粒悬浮在较低位置. 由于这种悬浮高度的差异, 不同尺寸尘埃颗粒在其各自悬浮高度上受到的棘轮势的不对称取向相反, 这种棘轮势取向差异直接决定了不同尺寸的尘埃颗粒沿棘轮通道朝相反方向流动. 本文研究结果从根本上阐明了尘埃等离子体金属直棘轮中尘埃颗粒整流的机制, 为进一步研究双分散尘埃颗粒分离奠定了理论基础, 同时促进了等离子体物理和非平衡统计物理的交叉融合, 对解决芯片制造工艺中的尘埃污染问题也具有重要意义.
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图 1 典型框架核酸结构: DNA瓦块和DNA折纸结构 (a) DNA瓦块组装成的二维晶格[28]; (b) DNA四面体[20]; (c) 类富勒烯结构[21]; (d) DNA折纸设计图及几种二维平面折纸结构[22]; (e) 球形[40]、花鸟图案[42]和兔子[41]线框DNA折纸结构; (f) DNA纳米花瓶结构[43]; (g) 16个折纸模块组成的蒙娜丽莎图案[50]
Fig. 1. Typical FNAs: DNA tile and DNA origami: (a) DNA four-way junction[28]; (b) DNA tetrahedron[20]; (c) DNA buckyball self-assembled by three-point-star DNA tiles[21]; (d) 2D DNA origami structures[22]; (e) sphere[40], flower-and-bird pattern[42] and bunny-shape[41] wireframe DNA origami structures; (f) nanoflask DNA origami structure with complex curvatures[43]; (g) a Mona Lisa pattern self-assembled by 16 DNA origami tiles[50].
图 2 框架核酸介导纳米颗粒组装 (a) DNA瓦块介导AuNPs组装成二维阵列[60]; (b) 三角形DNA纳米管封装的AuNP线[62]; (c) DNA折纸模块介导AuNPs形成平面阵列[63]; (d) DNA单链编码的AuNPs组装成分支状类分子结构[65]
Fig. 2. FNAs-directed nanoparticles assembly: (a) 2D AuNP arrays self-assembled by DNA tiles [60]; (b) AuNP lines size-selective encapsulated within triangular DNA nanotubes[62]; (c) 2D AuNP arrays directed by DNA origami tiles[63]; (d) branched molecule-like structures self-assembled by single-stranded DNA encoded AuNPs[65].
图 3 框架核酸介导原位生长 (a) 三角形DNA折纸上定点金属化形成银纳米簇[69]; (b) DNA折纸上选择性金属化构建8字形图案[70]; (c) DNA-二氧化硅复合材料的制备[71]; (d) DNA折纸上定点合成“i”形二氧化硅纳米结构[72]
Fig. 3. FNAs-directed in-situ growth of nanomaterials: (a) Silver nanoclusters synthesized on DNA origami[69]; (b) selective DNA condensation and metallization on DNA origami for fabricating a digit 8 pattern[70]; (c) DNA origami silicification diatom-mimicking structures[71]; (d) site-specific synthesis of “i-pattern” silica nanostructure on DNA origami[72].
图 4 框架核酸构建单分子反应器 (a) DNA 折纸上单分子化学键断裂反应[74]; (b) DNA折纸上光诱导多巴胺聚合反应[77]; (c) DNA折纸上酶通路调控系统[78]; (d) DNA纳米管中GOx和HRP的酶级联反应[79]; (e) DNA机器可逆调控酶级联反应[80]
Fig. 4. FNAs used for single molecule reactors: (a) Single-molecule chemical cleavage reactions on DNA origami[74]; (b) light-triggered polydopamine formation on DNA origami[77]; (c) enzyme pathway regulation system on a rectangular DNA origami platform[78]; (d) bienzyme cascade of GOx and HRP in a DNA origami nanotube[79]; (e) reversible regulation of enzyme cascade reaction by a DNA machine[80].
图 5 框架核酸构建单分子传感器 (a) DNA 折纸上设计的V形探针检测目标RNA[84]; (b) 字母图案的DNA折纸用于SNP检测[85]; (c) DNA四面体探针检测目标DNA[87]; (d) AuNP二聚体检测染料分子的SERS信号[88]; (e) AuNP四聚体对SERS信号的单分子水平定点、定量检测[89]
Fig. 5. FNAs used for single molecule sensing: (a) Detection of the target RNA by hybridization with V-shaped probe stretched from a DNA origami[84]; (b) SNP detection with alphabetic patterned origami structures [85]; (c) recognition of the target DNA with a DNA tetrahedral structured probe [87]; (d) DNA origami-templated AuNP dimers for SERS[88]; (e) DNA origami-templated tetrameric Au nanoclusters for quantizing single-molecule SERS[89].
图 6 框架核酸用于分子装载和输运 (a) DNA 折纸上的分子装配线[93]; (b) 电场驱动DNA纳米机械臂旋转并使金纳米棒运动[95]; (c) 凝血酶功能化的DNA纳米机器人[97]; (d) 3种用于经皮给药的DNA四面体结构[98]
Fig. 6. FNAs used for cargos loading and transporting: (a) Molecular assembly line on DNA origami[93]; (b) electrically actuated rotation of a nanorobotic arm, moving a gold nanorod[95]; (c) DNA origami nanocapsule actuated by changing pH[97]; (d) 3DNA tetrahedrons for transdermal drug delivery[98].
图 7 框架核酸的纳米光学应用 (a) 基于DNA四面体的光流体激光器实验装置[101]; (b) DNA-PAINT[102]; (c) DNA折纸上线性排列的AuNPs产生光波导[103]; (d) AuNPs在DNA折纸上的左旋和右旋排列[104]; (e) 四面体DNA折纸组装的金纳米棒手性超分子[105]; (f) 金纳米棒在DNA折纸上的动态行走[106]
Fig. 7. FNAs used for nanophotonics: (a) Optofluidic lasers based on a DNA tetrahedron[101]; (b) DNA-PAINT [102]; (c) waveguide on the line of AuNPs arranged by a DNA origami[103]; (d) AuNP helices on DNA origami[104]; (e) tetrahedral DNA origami-templated plasmonic metamolecules[105]; (f) Au nanorod walking on DNA origami[106].
图 8 框架核酸构建纳电子器件 (a) DNA折纸到SiO2基底的直接图案转移[114]; (b) 聚合物线在DNA折纸上形成的“U”形图案[115]; (c) DNA瓦块组装AuNP构建单电子晶体管[116]; (d) DNA折纸模板制备高度致密的CNT平行阵列[117]
Fig. 8. FNAs used for nanoelectronics: (a) Pattern transferring from DNA origami into SiO2[114]; (b) polymer binding to the DNA origami with a “U” shaped pattern[113]; (c) DNA tile-templated single electron nanoelectronics[116]; (d) CNT alignment based on trench-like DNA templates[117].
图 9 框架核酸构建信息处理器件 (a) DNA 折纸分子计算器[122]; (b) DNA单分子巡航机器人解迷宫[123]; (c) DNA折纸加密系统[124]; (d) DNA折纸多米诺阵列编码信息[125]
Fig. 9. FNAs used for information processing: (a) DNA origami calculator[122]; (b) single-molecule DNA navigator for solving maze on the 2 D origami[123]; (c) DNA origami cryptography system[124]; (d) DNA origami domino array for coding information[125].
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