共轭聚合物单分子构象和能量转移特性研究

利用基于宽场显微光学系统的单分子散焦成像技术测量了不同构象poly[2,7-(9,9-dioctylfluorene)-alt-4,7-bis(thiophen-2-yl)benzo-2,1,3-thiadiazole](PFO-DBT)共轭聚合物单分子的光物理与动力学特性.通过分析共轭聚合物单分子的荧光轨迹和对应的发射偶极取向变化识别共轭聚合物单分子发光单元,发现延伸构象下的单分子呈现多发色团发光特性,而折叠构象下的单分子保持高效链间能量转移,呈现单个发色团发光特性.共轭聚合物单分子构象对能量转移效率的影响可用于研究基于共轭聚合物的光电器件和分子器件.     

共轭链对具有特殊电荷转移结构分子超极化率的影响

近年来实验发现扭曲型分子内电荷转移(TICT)分子具有独特的分子内电荷转移机理和不同寻常的NLO响应系数.本文在MP2/6-311++G(d,p)水平上,结合有限场方法系统探讨了不同共轭链及共轭链长度对TICT分子一阶超极化率β的影响,并与传统D-π-A分子相比较.研究表明,共轭链对TICT分子与传统D-π-A分子β影响不同,且随着共轭链增长,TICT分子β提高更为显著.特别是共轭链为苯环的P4分子,当苯环重复单元数n=3时,其β远远大于其它具有不同共轭链的分子.     

基于库仑阻塞原理的多值存储器

设计了一种基于库仑阻塞原理的新型单电子多值存储器.器件包括两个多隧穿结结构和一个单电子晶体管，其中单电子晶体管起到一个静电计的作用来实现数据的读取.两个隧穿结库仑阻塞区域的大小不同使得器件具有三个稳定的存储状态.利用这个原理可以制备出多值的动态随机存储器和非挥发性的随机存储器.这种低功耗的单电子多值存储器可以实现信息的超高密度存储. 关键词： 库仑阻塞 单电子晶体管     

聚乙烯醇中的紫外偏振线性聚炔分子（英文）

本文通过研究共轭线性碳链分子,聚炔H(C≡C)_nH(n=5～7)的电子吸收带,设计了适用于UV的光偏振膜.激光烧蚀的聚炔分子被分散在聚乙烯醇膜中.结构各向异性的性质使得多炔分子的UV吸收跃迁偶极子与分子轴平行,并且吸收仅发生在沿着分子轴具有电子矢量幅度的电磁波上.多炔分子在固体聚乙烯醇膜中作为特定波长入射光的偏振分量之一的选择性吸收剂.使用可旋转的偏振UV光研究包含聚炔分子的拉伸聚乙烯醇膜的吸收强度的角度依赖性,并根据线性二向色性理论中有序参数进行分析.     

异构二芳基乙烯分子结低偏压电导机制的第一性原理研究

本文用结合密度泛函理论的非平衡格林函数方法研究了具有开环和闭环两种同分异构体的二芳基乙烯衍生物分子的结构-特性关系. 该功能分子通过末端的吡啶基团连接到取向沿(111)方向的金电极. 计算结果表明，异构体分子结的不同低偏压电导主要是由于它们具有不同的电子结构. 两种构型分子结的低偏压导电都主要来自于电子隧穿最低未占据分子轨道(LUMO). 由于具有扩展的单双键交替共轭结构，闭环构型分子具有更好的导电通道. 通过计算分子结在平衡状态下的电子转移，可发现更多电子转移到闭环构型分子，导致了其LUMO能量更靠近费米能级，从而有利于低偏压下的导电性能. 结果有助于理解二芳基乙烯分子及其衍生物分子的低偏压电导机制，也为设计更高性能的同类分子开关提供理论依据.     

一种新型双共轭链分子非线性光学性质的理论研究

对实验室合成的双共轭链分子1,4-二(4-二乙胺基苯乙烯基)-2-［4-(N-甲基-N-羟乙基)氨基-4′-硝基偶氮苯］-5-己烷氧基苯(BSBAB)及合成它的单共轭链分子的单光子和双光子吸收特性在从头计算的基础上利用密度泛函理论进行了研究.分子BSBAB的优化结构显示，组成该分子的横链和纵链除了保持各自的共轭面外，几近相互垂直.因此，分子BSBAB较好地继承了两个单共轭链分子的光学特性.计算结果表明，在低能量范围内，分子BSBAB具有三个双光子吸收峰，分别来自于两个单共轭链分子以及两者的耦合作用.从理论上证明了双共轭链分子BSBAB是一种具有宽带强双光子吸收的分子材料.理论结果和实验结果符合得较好.在HF水平上的响应函数方法进一步证实了有限态求和方法计算结果的可靠性.还给出了电荷转移态的电荷迁移过程. 关键词： 双光子吸收 双共轭链有机分子 非线性光学     

激光溅射Cu等离子体与气相CH3CN团簇的反应

用激光溅射 -分子束技术研究了Cu等离子体与乙腈团簇的气相反应 .观察到Cu+ (CH3 CN) n、CH2 CN+ (CH3 CN) n、H+ (CH3 CN) n 和CH3 CHCN+ (CH3 CN) n 四个种类的团簇离子 .考察了等离子体作用于脉冲分子束的不同位置 ,对团簇产物的种类和尺寸大小的影响 .实验结果表明 ,Cu+ (CH3 CN) n 是由Cu+ 与乙腈团簇直接缔合而成 ,CH2 CN+ (CH3 CN) n、H+ (CH3 CN) n 主要是激光等离子体中的电子与乙腈团簇碰撞电离产生的 ,而CH3 CHCN+ (CH3 CN) n 是由乙腈团簇离子内的离子 分子反应生成的 .     

共轭链对具有特殊电荷转移结构分子超极化率的影响

近年来实验发现扭曲型分子内电荷转移（TICT）分子具有独特的分子内电荷转移机理和不同寻常的NLO响应系数。本文在MP2/6-311++G(d,p)水平上,结合有限场方法系统探讨了不同共轭链及共轭链长度对TICT分子一阶超极化率β的影响,并与传统D-π-A分子相比较。研究表明,共轭链对TICT分子与传统D-π-A分子β影响不同,且随着共轭链增长,TICT分子β提高更为显著。特别是共轭链为苯环的P4分子,当苯环重复单元数n=3时,其β远远大于其它具有不同共轭链的分子。     

单分子器件电输运中基于量子干涉效应的调控策略

单分子器件电输运中的量子干涉效应是电子在分子独立的轨道能级内传输时因保持量子相干性,从而在不同能级之间发生相互干涉的现象.这种现象导致了电子在单分子器件内透射概率的增加或减小,在实验中体现为单分子器件电导值的升高或降低.近些年,利用量子干涉效应对不同的单分子器件进行调控在实验中被证实是有效的调控手段,如对单分子开关、单分子热电器件、单分子自旋器件等器件性能的调控.本文介绍了量子干涉效应的相关理论与预测、实验观测与证实,以及其在不同单分子器件上的调控作用.     

一维介观结链中的双电荷孤子

采用半经典模型研究了一维介观结链中两个岛上各存在一个剩余电子时的电势分布,发现在一维介观链中存在双电荷孤子.双电荷孤子的主要特征是它的电势峰发生了劈裂,形成双峰,两峰在通常情况下不等高.研究了双电荷孤子电势峰和阈电压对一维介观结链结构参数的依赖关系.提出了研究双电荷孤子的等效单电荷孤子方法,表明在等效电荷区域,双电荷孤子的电势分布与等效单电荷孤子在同一区域的电势分布相同. 关键词： 双电荷孤子 介观结 单电子效应     

Antiresonance and decoupling in electronic transport through parallel-coupled quantum-dot structures with laterally-coupled Majorana zero modes

We theoretically investigate the electronic transport through a parallel-coupled multi-quantum-dot system, in which the terminal dots of a one-dimensional quantum-dot chain are embodied in the two arms of an Aharonov–Bohm interferometer. It is found that in the structures of odd(even) dots, all their even(odd) molecular states have opportunities to decouple from the leads, and in this process antiresonance occurs which are accordant with the odd(even)-numbered eigenenergies of the sub-molecule without terminal dots. Next when Majorana zero modes are introduced to couple laterally to the terminal dots, the antiresonance and decoupling phenomena still co-exist in the quantum transport process. Such a result can be helpful in understanding the special influence of Majorana zero mode on the electronic transport through quantum-dot systems.     

B/N掺杂对于石墨烯纳米片电子输运的影响

选用锯齿(zigzag)型石墨烯纳米片为研究对象, Au作为电极, 分子平面与Au的(111)面垂直, 并通过末端S原子化学吸附于金属表面, 构成两种分子器件: 一种是在纳米片的边缘掺杂N(B)原子, 发现电流-电压具有非线性行为, 但是整流系数较小, 特别是掺杂较多时, 整流具有不稳定性; 另一种是用烷链把两个石墨烯片连接, 在烷链附近和石墨烯片的边缘进行N(B)掺杂, 发现在烷链附近掺杂具有较大的整流, 但是掺杂的原子个数和位置会影响整流性能. 研究表明: 整流主要为正负电压下分子能级的移动方向和空间轨道分布不同导致. 部分体系中的负微分电阻现象主要由于偏压导致能级移动和透射峰形态的改变, 并且在某些偏压下主要透射通道被抑制而引起. 关键词： 石墨烯纳米片 电子输运 整流行为 非平衡格林函数方法     

Electronic transport properties of silicon chains sandwiched between graphene electrodes: first-principles study

The effects of orientation and silicon chain length on the electronic transport properties for linear silicon chains sandwiched between two graphene electrodes are investigated by using non-equilibrium Green’s functions combined with density functional theory. Our results demonstrate that the conductance of single silicon chains can hardly be affected by its orientation, as there is negligible difference between the conductance of tilted and un-tilted chains, and the conductance is impacted greatly by the length of chains, i.e. the transmission coefficient is doubled for double chains. The equilibrium conductance of single silicon chains shows even-odd oscillating behavior, and its tendency decreases with the increase of the chain length. The non-equilibrium electronic transport properties for all types of chains are also calculated, and all current–voltage curves of silicon chains show a linear character. The frontier molecular orbitals, the total and projected density of states are used to analyse the electronic transport properties for all types of chains.     

Electron transport in graphene nanoribbons under a central potential modulation

We study electron transport in graphene nanoribbons (GNs) under a one-dimensional central potential. Two kinds of structures are considered: armchair-edged GN (AGN) where a central potential is applied on the central dimer chain, and zigzag-edged GN (ZGN) where a potential is applied on the central zigzag chain. Both nanoribbons show unique electronic structure and interesting transport properties under potential modulation. Without considering edge effect, a metallic AGN is still metallic after potential modulation. However, if the edge effect is considered, an AGN under potential modulation can be either semiconducting or metallic depending on the potential strength. The AGN transits from semiconducting to metallic and then to semiconducting again with the potential increase. As to ZGN, the potential on the central zigzag chain also greatly affect the quantum conductance. A ZGN will transit from metallic to semiconducting as the potential strength exceeds critical value. All transitions of AGN and ZGN are correlated with the localized state on the central potential chain which induces a quantum channel along the chain.     

单空位缺陷对石墨纳米带电子结构和输运性质的影响

基于第一性原理电子结构和输运性质计算,研究了单空位缺陷对单层石墨纳米带(包括zigzag型和armchair型带)电子性质的影响.研究发现,单空位缺陷使石墨纳米带在费米面上出现一平直的缺陷态能带;单空位缺陷的引入使zigzag型半导体性的石墨纳米带变为金属性,这在能带工程中有重要的应用价值;奇数宽度的armchair型石墨纳米带表现出金属特性,有着很好的导电性能,同时,偶数宽度的armchair型石墨带虽有金属性的能带结构,但却有类似半导体的伏安特性;单空位缺陷使得奇数宽度的armchair石墨纳米带导电 关键词： 石墨纳米带 单空位缺陷 电子结构 输运性质     

Antiresonance of electron tunneling through a quantum dot array

Electronic transport through a one-dimensional quantum dot array is theoretically studied. In such a system both electron reservoirs of continuum states couple with the individual component quantum dots of the array arbitrarily. When there are some dangling quantum dots in the array outside the dot(s) contacting the leads, the electron tunneling through the quantum dot array is wholly forbidden if the electron energy is just equal to the molecular energy levels of the dangling quantum dots, which is called as antiresonance of electron tunneling. Accordingly, when the chemical potential of the reservoir electrons is aligned with the electron levels of all quantum dots, the linear conductance at zero temperature vanishes if there are odd number dangling quantum dots; Otherwise, it is equal to 2e²/h due to resonant tunneling if the total number of quantum dots in the array is odd. This odd–even parity is independent of the interdot and the lead–dot coupling strength.     

The influence of coupling between chains on the conductivity of atomic carbon chains

This work presents a theoretical investigation on the electronic properties of double atomic carbon chains bridging graphene electrodes with density functional theory in combination with non-equilibrium Green's function. The influence of strain on the conductance of atomic carbon chains is significant. However, the coupling effect between adjacent chains dominates the intrinsic transport of double atomic carbon chains. For the coupled double atomic chains, the electron conductance of even-numbered atomic chains is significantly enhanced, while the electron conductance of odd-numbered atomic chains decreases to a certain degree, and the dependence of the conductance of double atomic chains on electrode configuration is stronger than the corresponding single atomic chain. More intriguingly, the coupled double atomic chains exhibit excellent spin-filtering properties with antiparallel spins on two electrodes. The current spin polarization stems from the coupling-induced changes of electron density and band offset reaches 100%. The coupled double atomic carbon chains have great potential application in spintronic devices and carbon-based field-effect transistors.     

Effect of crystallographic orientations on transport properties of methylthiol-terminated permethyloligosilane molecular junction

The understanding of the influence of electrode characteristics on charge transport is essential in the field of molecular electronics. In this work, we investigate the electronic transport properties of molecular junctions comprising methylthiol-terminated permethyloligosilanes and face-centered crystal Au/Ag electrodes with crystallographic orientations of (111) and (100), based on the ab initio quantum transport simulations. The calculations reveal that the molecular junction conductance is dominated by the electronic coupling between two interfacial metal-S bonding states, which can be tuned by varying the molecular length, metal material of the electrodes, and crystallographic orientation. As the permethyloligosilane backbone elongates, although the σ conjugation increases, the decreasing of coupling induced by the increasing number of central Si atoms reduces the junction conductance. The molecular junction conductance of methylthiol-terminated permethyloligosilanes with Au electrodes is higher than that with Ag electrodes with a crystallographic orientation of (111). However, the conductance trend is reversed when the electrode crystallographic orientation varies from (111) to (100), which can be ascribed to the reversal of interfacial coupling between two metal-S interfacial states. These findings are conducive to elucidating the mechanism of molecular junctions and improving the transport properties of molecular devices by adjusting the electrode characteristics.     

Transverse field effect in graphene ribbons

It is shown that a graphene ribbon, a ballistic strip of carbon monolayer, may serve as a quantum wire whose electronic properties can be continuously and reversibly controlled by an externally applied transverse voltage. The electron bands of armchair-edge ribbons undergo dramatic transformations: The Fermi surface fractures, Fermi velocity and effective mass change sign, and excitation gaps are reduced by the transverse field. These effects are manifest in the conductance plateaus, van Hove singularities, thermopower, and activated transport. The control over one-dimensional bands may help enhance effects of electron correlations, and be utilized in device applications.     

基于石墨烯电极的蒽醌分子器件开关特性

研究了基于石墨烯电极的蒽醌分子器件的开关特性.分别选取了锯齿型和扶手椅型的石墨烯纳米带作为电极,考虑蒽醌基团在氧化还原反应下的两种构型,即氢醌(HQ)分子和蒽醌(AQ)分子,构建了双电极分子结,讨论了氧化还原反应和不同的电极结构对蒽醌分子器件开关特性的影响.研究发现,无论是锯齿型石墨烯电极还是扶手椅型石墨烯电极,HQ构型的电流都明显大于AQ构型的电流,即在氧化还原反应下蒽醌分子呈现出显著的开关特性.同时,当选用锯齿型石墨烯电极时其开关比最高能达到3125,选用扶手椅型石墨烯电极时开关比最高能达到1538.此外,当HQ构型以扶手椅型石墨烯为电极时,在0.7-0.75 V之间表现出明显的负微分电阻效应.因此该系统在未来分子开关器件领域具有潜在的应用价值.