Organic magnetoresistance and spin diffusion in organic semiconductor thin film devices

We review recent work in the field of organic spintronics, focusing on our own contributions to this field. There are two principle magnetoresistance effects that occur in organic devices. (i) Organic magnetoresistance (OMAR), which occurs in nonmagnetic organic semiconductor devices. For example, in devices made from the prototypical small molecule Alq₃ OMAR reaches values of 10% or more at room temperature. (ii) Organic spin‐valve effects that occur in devices that employ ferromagnetic electrodes for spin‐polarized current injection and detection. We undertake an analysis of these two types of magnetoresistance with the goal of identifying the dominant spin‐scattering mechanism. Analysis of OMAR reveals that hyperfine coupling is the dominant spin‐coupling mechanism. Spin–orbit coupling, on the other hand, is important only in organic semiconductor materials containing heavy atoms. We explore the reasons why spin–orbit coupling is relatively unimportant in hydrocarbon materials. Next, we present a theory for spin diffusion in disordered organic semiconductors based on hyperfine coupling, taking into account a combination of incoherent carrier hopping and coherent spin precession in the random hyperfine magnetic fields. We compare our findings with experimental values for the spin‐diffusion length. Finally, we demonstrate a criterion that allows the determination whether the organic spin‐valves operate in the tunneling or injection regimes. (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

有机半导体外延生长的扫描隧道显微镜研究

有机半导体薄膜的光、电等性质取决于有机分子的取向以及长程有序性.研究有机半导体的生长机理以及内在驱动力是一个重要环节.文章通过两个典型生长体系,perylene 在Ru(0001)表面上的生长和tetracene在Ag(110)表面上生长过程的介绍,给出了形成有机半导体晶化薄膜的可能性以及决定其有序生长的内在驱动力.对于perylene 在Ru(0001)表面上的生长,决定其过程的主要驱动力是分子间的相互排斥作用,在单分子层时,由于这种相互作用导致形成Ru(0001)- 12×12-8 perylene有序超结构.而对于tetracene/Ag(110)体系,决定生长的驱动力主要表现为相互吸引作用,因此,在小于单分子层时,tetracene呈有序的岛状生长;而当tetracene膜的厚度大于单分子层时,呈逐层生长模式,并形成具有正交晶系结构的晶化薄膜.     

电声子相互作用对量子点分子中单电子隧穿的影响

研究了双量子点系统中的电子隧穿动力学过程，在考虑电子与声子相互作用的情况下用基于 正则变换的微扰方法解析地得到了电子动态隧穿电流的表达式. 并且详细分析电子与声子耦 合引起的退相干问题，在此基础上指出了可能的退耦机理. 关键词： 电声子相互作用 双量子点 隧穿     

表/界面水的扫描探针技术研究进展

表面和界面水在自然界、人们的日常生活以及现代科技中无处不在.它在物理、化学、环境学、材料学、生物学、地质学等诸多基础学科和应用领域起到至关重要的作用.因此,表面和界面水的功能与特性的研究,是水基础科学的一项核心任务.然而,由于水分子之间氢键相互作用的复杂性,及其与水-固界面相互作用的竞争,使得表(界)面水对于局域环境的影响非常敏感,往往需要深入到分子层次研究其微观结构和动力学过程.近年来,新型扫描探针技术的发展使得人们可以在单分子甚至亚分子尺度上对表(界)面水展开细致的实空间研究.本文着重介绍几种代表性的扫描探针技术及其在表(界)面水体系中的应用,包括:超高真空扫描隧道显微术、单分子振动谱技术、电化学扫描隧道显微术和非接触式原子力显微术.此外,本文还将对表(界)面水扫描探针技术研究面临的挑战和未来发展方向进行了展望.     

Force spectroscopy of single multidomain biopolymers: A master equation approach

Experiments using atomic force microscopy for unfolding single multidomain biopolymers cover a broad range of time scales from equilibrium to non-equilibrium. A master equation approach allows to identify and treat coherently three dynamical regimes for increasing linear ramp velocity: i) an equilibrium regime, ii) a transient regime where refolding events still occur, and iii) a saw-tooth regime without any refolding events. For each regime, analytical approximations are derived and compared to numerically investigated examples. We analyze in the framework of this model also a periodic experimental protocol instead of a linear ramp. In this case, a major simplification arises if the dynamics can be restricted to an effectively two-dimensional subspace. For transitions with an intermediate meta-stable state, like Immunoglobulin27, a refined model allows to extract previously unknown molecular parameters related to this meta-stable state.     

双势阱中冷原子的关联隧穿

研究了在不同的相互作用和隧穿耦合强度比值情况下双势阱中冷原子的隧穿现象.两格点Bose-Hubbard模型不能完全解释实验.为此,对此模型做了高阶修正.取双势阱的基态和第一激发态作基矢,写出哈密顿量的表示,解释了用两格点Bose-Hubbard模型分析实验时参数不能定量符合的原因.另外,通过计算两阱中原子纠缠度的变化,结合三态上原子布居数分布,直观描述了整个隧穿过程.     

双势阱中冷原子的关联隧穿

研究了在不同的相互作用和隧穿耦合强度比值情况下双势阱中冷原子的隧穿现象.两格点Bose-Hubbard模型不能完全解释实验.为此,对此模型做了高阶修正.取双势阱的基态和第一激发态作基矢,写出哈密顿量的表示,解释了用两格点Bose-Hubbard模型分析实验时参数不能定量符合的原因.另外,通过计算两阱中原子纠缠度的变化,结合三态上原子布居数分布,直观描述了整个隧穿过程.     

界面势垒对碳纳米管场发射特性的影响

以界面势垒对碳纳米管(CNT)场发射的影响为研究目的,在硅衬底上引进很薄的二氧化硅层,以二氧化硅层作为绝缘势垒,然后在二氧化硅界面层上直接生长CNT,来研究二氧化硅绝缘势垒层对CNT场发射的影响。场发射结果为:Fowler-Nordheim(F-N)曲线分为两部分,高电场下偏离F-N曲线并趋于饱和。在双势垒模型的基础上,从电场在两势垒上的分布不同及电子在两势垒上的隧穿几率不同,理论上分析了界面势垒对场发射的影响:低电场下电子在界面势垒的隧穿几率大于在表面势垒的隧穿几率,界面势垒对场发射不起阻碍作用,场发射遵守F-N规律;高电场下电子在界面势垒的隧穿几率小于在表面势垒的隧穿几率,场发射偏离F-N规律。理论对实验结果进行了合理的解释。     

联苯二胺分子器件电输运特性的取代效应

在第一性原理基础上,理论研究了苯环上含有不同取代物的四个联苯分子的电输运特性.计算结果表明,当苯环上的氢被取代时,联苯分子的两个苯环之间的扭转角增大.分子结的电导随苯环间扭转角的增加而减少,且电导值与扭转角余弦平方成线性关系.在低偏压下,分子结的电输运机制是电子通过π轨道的隧穿过程.计算结果与实验结果符合的较好.     

Structural properties of Cu clusters on Si(1 1 1):Cu2Si magic family

Basing on the results of the scanning tunneling microscopy (STM) observations and density functional theory (DFT) calculations, the structural model for the Cu magic clusters formed on Si(1 1 1)7 × 7 surface has been proposed. Using STM, composition of the Cu magic clusters has been evaluated from the quantitative analysis of the Cu and Si mass transport occurring during magic cluster converting into the Si(1 1 1)‘5.5 × 5.5’-Cu reconstruction upon annealing. Evaluation yields that Cu magic cluster accommodates 20 Cu atoms with 20 Si atoms being expelled from the corresponding 7 × 7 half unit cell (HUC). In order to fit these values, it has been suggested that the Cu magic clusters resemble fragments of the Cu₂Si-silicide monolayer incorporated into the rest-atom layer of the Si(1 1 1)7 × 7 HUCs. Using DFT calculations, stability of the nineteen models has been tested of which five models appeared to have formation energies lower than that of the original Si(1 1 1)7 × 7 surface. The three of five models having the lowest formation energies have been concluded to be the most plausible ones. They resemble well the evaluated composition and their counterparts are found in the experimental STM images.