连接构型对铬卟啉分子自旋过滤效应的调控

采用第一性原理方法对不同连接构型的铬卟啉分子电子自旋输运性质进行计算分析.结果表明，对角连接构型的铬卟啉分子在0～0.2 V偏压区间范围内的自旋极化率高达95%以上，水平连接构型的导电性能比对角连接高约1个数量级.说明改变铬卟啉分子连接构型，可以改变电子自旋前线分子轨道分布和输运路径，从而实现其自旋过滤效应，对基于不同连接构型的铬卟啉分子器件的电子自旋输运性质进行有效调控.     

三终端量子点环中的自旋极化输运

利用非平衡态格林函数方法,研究了一个存在局域Rashba自旋轨道耦合作用的三电极量子点环结构中的电子输运性质.结果发现,Rashba自旋轨道耦合作用引起的自旋相关的量子干涉效应能够在电极中产生自旋流.这种自旋流的大小、方向以及自旋极化度等性质可以通过纯电学手段改变系统参数来加以调控.在适当选择这些参数时,电极中甚至可以产生完全自旋极化流或纯自旋流.这些效应说明我们所研究的系统可用来设计纯电学的自旋流产生装置.     

有机自旋电子学研究进展

本文从铁磁有机器件与非磁有机器件两方面介绍了近年来有机自旋电子学研究进展,理论上探讨了有机功能材料内的自旋极化注入与输运、自旋的微观动力学过程以及调控载流子的自旋取向对器件整体性能的影响。针对最近发现的有机强磁效应,从实验与理论两方面作了系统的阐述。     

正交电场作用型自旋场效应管的自旋极化控制

研究了电场调控型自旋场效应管的量子输运过程.该场效应管主要由双正交电场和Rashba自旋轨道耦合共同调制.运用散射矩阵方法并结合介观体系的相关输运理论,揭示了自旋场效应管在各参数调控下的自旋量子输运过程,其自旋输运规律可由相关理论给予解释.数值计算表明,与平行电场相比,对于自旋轨道耦合型自旋场效应管的量子输运,垂直电场的调制能够导致更加明显的自旋翻转.     

具有自旋-轨道耦合作用的二维介观电子气中的自旋累积效应研究

建立了在含自旋-轨道耦合相互作用的二维介观多端格子模型中求解散射波函数，进而在Landauer-Buttiker框架中得到计算多端的电导和自旋电导，以及任意非平衡局域物理量（如电流驱动之下的非平衡自旋累积）的一般方法．作为散射波函数法的一个直接应用，我们研究了具有Rashba型自旋-轨道耦合的二维电子气的二端结构，在给定电流密度条件下，我们得到线性输运区的非平衡自旋累积效应的结果，发现与其它的理论结果和最近的实验结果是定性一致的．     

量子点体系中自旋过滤、自旋流产生和自旋注入

自旋电子学是一门新兴的交叉学科,其中心主题就是对固体电子系统中电子的自旋自由度进行有效地操作和控制.量子点体系中的自旋效应近期受到了理论和实验较多的关注.本文着重介绍了自旋轨道耦合效应对量子点体系输运性质的影响,探讨了怎样利用自旋轨道耦合效应来实现对自旋的有效过滤和纯自旋流产生.基于四铁磁端双量子点体系中电子的交换相互作用机制,指出了一种可以显著提高从铁磁金属到半导体量子点自旋注入效率的新方法.     

四端介观量子网络中电子自旋的相干输运性质

采用解线性方程组的方法,研究了存在磁通时,四端介观量子网络中电子自旋的相干输运性质。该四端网络由具有Rashba自旋-轨道耦合互作用的量子线构成,数值计算了自旋电导对约化磁通和自旋-轨道耦合强度的依赖关系。计算结果表明:该网络中的自旋相干输运性质由约化磁通和Rashba自旋-轨道耦合之间的相互作用共同决定。这种结构中,一些端可以作为栅极控制其他端的自旋流,该四端多通道网络结构为调控电子自旋的相干输运提供了更多的选择。     

在Rashba和Dresselhaus自旋轨道耦合相互作用下二端双通道中的局域自旋极化研究

研究二端双通道结构中同时存在Rashba和Dresselhaus两种自旋轨道耦合相互作用情况下的电子局域自旋极化.本结构中所产生的局域自旋极化是由量子干涉效应和自旋轨道耦合共同导致的,因此可以通过调节结构参数和门电压的大小来改变局域自旋极化的大小.在适当选取某些参数的情况下.局域自旋极化可以达到0.33,可以用于自旋过滤器和信息储存器件.     

自旋轨道耦合与自旋霍尔效应?

从巨磁阻效应正式拉开自旋电子学的序幕开始,如何控制和操纵电子的自旋自由度在学术界和工业界掀起了巨大的研究浪潮,如何产生并测量自旋流也是自旋电子学面临的重大挑战.自旋轨道耦合为自旋电子学提供了利用全电学来控制自旋的物理基础,由自旋轨道耦合引起的自旋霍尔效应则为自旋电子学提供了产生较大纯自旋流的方法.本文从1879年Edwin Hall发现的那个迷人的效应谈起,同时从自旋轨道耦合的起源来认识自旋霍尔效应,进一步探讨了如何利用其逆效应来探测自旋霍尔效应及自旋流,并简单总结了与自旋霍尔效应相关的部分新效应及新应用.     

四端介观量子网络中电子的相干输运性质

采用解线性方程组的方法研究了同时存在磁通和Rashba自旋一轨道耦合的四端介观量子网络中电子的相干输运性质．计算结果表明,该量子网络中电子的相干输运是量子干涉和自旋进动的联合效应。这种四端多通道结构为调制电子的相干输运提供了更多的选择。     

方形(S,S,S,S)手性环芳烃的紫外吸收光谱和圆二色谱的量子化学研究

采用密度泛函理论研究了方形(S,S,S,S)手性环芳化合物的紫外吸收光谱(UV-Vis)和电子圆二色谱(ECD),从微观角度分析了产生UV-Vis、ECD谱吸收的分子轨道电子跃迁情况,解释了分子结构与光学活性的关系.     

X-ray magnetic circular dichroism： Orbital and spin moments of iron single-crystal thin film deposited on MgO substrate

X-ray magnetic circular dichroism in absorp-tion of the single-crystal iron layer deposited epitaxially on MgO substrate is studied. Spin and orbital moment, 0.069and 2.33μs, respectively, are calculated in terms of the XMCD sum rules. Our results are accordant to those published. Experiments show that the orbital moment would be decreased to that in bulk materials as iron film is thinned down, but spin moment changes little.     

Detection of magnetic circular dichroism using a transmission electron microscope

A material is said to exhibit dichroism if its photon absorption spectrum depends on the polarization of the incident radiation. In the case of X-ray magnetic circular dichroism (XMCD), the absorption cross-section of a ferromagnet or a paramagnet in a magnetic field changes when the helicity of a circularly polarized photon is reversed relative to the magnetization direction. Although similarities between X-ray absorption and electron energy-loss spectroscopy in a transmission electron microscope (TEM) have long been recognized, it has been assumed that extending such equivalence to circular dichroism would require the electron beam in the TEM to be spin-polarized. Recently, it was argued on theoretical grounds that this assumption is probably wrong. Here we report the direct experimental detection of magnetic circular dichroism in a TEM. We compare our measurements of electron energy-loss magnetic chiral dichroism (EMCD) with XMCD spectra obtained from the same specimen that, together with theoretical calculations, show that chiral atomic transitions in a specimen are accessible with inelastic electron scattering under particular scattering conditions. This finding could have important consequences for the study of magnetism on the nanometre and subnanometre scales, as EMCD offers the potential for such spatial resolution down to the nanometre scale while providing depth information--in contrast to X-ray methods, which are mainly surface-sensitive.     

贵金属/半导体异质结中的光致自旋电流效应研究

自旋电子材料因能同时对电子的自旋和电荷两个自由度实施操控,在构筑以低功耗、超高速、大容量和超宽带为特征的新一代信息处理技术中展现出巨大的应用潜力.然而,通过掺杂过渡金属元素和稀土离子而形成的传统稀磁半导体和钙钛矿锰氧化物往往因结构缺陷导致的居里温度不高、自旋磁矩和自旋极化率偏低等不足,阻碍了自旋电子材料的商业化应用.近年来,在高纯半导体上沉积贵金属薄膜所形成的贵金属/半导体异质结中,通过使用偏振光激发该类异质结可产生纯自旋电流.这种基于逆自旋霍尔效应(ISHE)、可在室温下运行的、非接触和非破坏型的自旋极化激励方法理论上可获得高于50%自旋极化率,引起了人们的广泛关注.文章主要介绍光致自旋电流形成机制和测试方法,以及入射光圆偏振度、光强、入射角度等参数对光致自旋注入效率的调控机理,介绍杂质介导和声子介导对光致自旋输运的贡献,最后提出增强光致自旋电子极化率的可行方案,可为揭示自旋载流子产生、注入和输运相关的自旋动力学核心科学问题以及研制高性能自旋电子器件提供有益的参考.     

Absolute configuration of chirally deuterated neopentane

The relationship between macroscopic chirality and chirality on the molecular level was unequivocally established in 1951 through anomalous X-ray scattering. Although this technique became the definitive method for determining the absolute configuration of a molecule, one important limitation of the approach is that the molecule must contain 'heavy' atoms (for example, bromine). The direct determination of absolute configurations for a wider range of molecules has recently become possible by measuring a molecule's vibrational optical activity. Here we show that instrumental advances in Raman optical activity, combined with quantum chemical computations, make it possible to determine the absolute configuration of (R)-[2H1, 2H2, 2H3]-neopentane. This saturated hydrocarbon represents the archetype of all molecules that are chiral as a result of a dissymmetric mass distribution. It is chemically inert and cannot be derivatized to yield molecules that would reveal the absolute configuration of the parent compound. Diastereomeric interactions with other molecules, optical rotation, and electronic circular dichroism are, in contrast to the well-known case of bromochlorofluoromethane, not expected to be measurable. Vibronic effects in the vacuum ultraviolet circular dichroism might reveal that the molecule is chiral, but the presence of nine rotamers would make it extremely difficult to interpret the spectra, because the spatial arrangement of the rotamers' nuclei resembles that of enantiomers. The unequivocal spectroscopic determination of the absolute configuration of (R)-[2H1, 2H2, 2H3]-neopentane therefore presented a major challenge, one that was at the very limit of what is possible.     

基于磁光材料的磁可调石墨烯多带吸收特性

为了改善石墨烯的吸收性能,基于石墨烯的磁光效应,提出了一种采用磁性材料构成的光子晶体异质结构。该光学结构可使石墨烯实现多带吸收。吸收带的数目可通过改变光子晶体的周期数来调节。利用4×4传输矩阵法数值研究了该光子晶体异质结构的相关参数对石墨烯吸收率的影响。结果表明:石墨烯的吸收特性表现出一定的磁圆二色性。但通过调节费米能量,在外磁场的作用,左旋圆偏振光和右旋圆偏振光均可具有较高的吸收率。研究结果为偏振光学领域石墨烯基新型光子学器件的设计制作提供了理论依据。     

Single-shot read-out of an individual electron spin in a quantum dot

Spin is a fundamental property of all elementary particles. Classically it can be viewed as a tiny magnetic moment, but a measurement of an electron spin along the direction of an external magnetic field can have only two outcomes: parallel or anti-parallel to the field. This discreteness reflects the quantum mechanical nature of spin. Ensembles of many spins have found diverse applications ranging from magnetic resonance imaging to magneto-electronic devices, while individual spins are considered as carriers for quantum information. Read-out of single spin states has been achieved using optical techniques, and is within reach of magnetic resonance force microscopy. However, electrical read-out of single spins has so far remained elusive. Here we demonstrate electrical single-shot measurement of the state of an individual electron spin in a semiconductor quantum dot. We use spin-to-charge conversion of a single electron confined in the dot, and detect the single-electron charge using a quantum point contact; the spin measurement visibility is approximately 65%. Furthermore, we observe very long single-spin energy relaxation times (up to approximately 0.85 ms at a magnetic field of 8 T), which are encouraging for the use of electron spins as carriers of quantum information.     

DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response

Matter structured on a length scale comparable to or smaller than the wavelength of light can exhibit unusual optical properties. Particularly promising components for such materials are metal nanostructures, where structural alterations provide a straightforward means of tailoring their surface plasmon resonances and hence their interaction with light. But the top-down fabrication of plasmonic materials with controlled optical responses in the visible spectral range remains challenging, because lithographic methods are limited in resolution and in their ability to generate genuinely three-dimensional architectures. Molecular self-assembly provides an alternative bottom-up fabrication route not restricted by these limitations, and DNA- and peptide-directed assembly have proved to be viable methods for the controlled arrangement of metal nanoparticles in complex and also chiral geometries. Here we show that DNA origami enables the high-yield production of plasmonic structures that contain nanoparticles arranged in nanometre-scale helices. We find, in agreement with theoretical predictions, that the structures in solution exhibit defined circular dichroism and optical rotatory dispersion effects at visible wavelengths that originate from the collective plasmon-plasmon interactions of the nanoparticles positioned with an accuracy better than two nanometres. Circular dichroism effects in the visible part of the spectrum have been achieved by exploiting the chiral morphology of organic molecules and the plasmonic properties of nanoparticles, or even without precise control over the spatial configuration of the nanoparticles. In contrast, the optical response of our nanoparticle assemblies is rationally designed and tunable in handedness, colour and intensity-in accordance with our theoretical model.     

Reconfigurable self-assembly through chiral control of interfacial tension

From determining the optical properties of simple molecular crystals to establishing the preferred handedness in highly complex vertebrates, molecular chirality profoundly influences the structural, mechanical and optical properties of both synthetic and biological matter on macroscopic length scales. In soft materials such as amphiphilic lipids and liquid crystals, the competition between local chiral interactions and global constraints imposed by the geometry of the self-assembled structures leads to frustration and the assembly of unique materials. An example of particular interest is smectic liquid crystals, where the two-dimensional layered geometry cannot support twist and chirality is consequently expelled to the edges in a manner analogous to the expulsion of a magnetic field from superconductors. Here we demonstrate a consequence of this geometric frustration that leads to a new design principle for the assembly of chiral molecules. Using a model system of colloidal membranes, we show that molecular chirality can control the interfacial tension, an important property of multi-component mixtures. This suggests an analogy between chiral twist, which is expelled to the edges of two-dimensional membranes, and amphiphilic surfactants, which are expelled to oil-water interfaces. As with surfactants, chiral control of interfacial tension drives the formation of many polymorphic assemblages such as twisted ribbons with linear and circular topologies, starfish membranes, and double and triple helices. Tuning molecular chirality in situ allows dynamical control of line tension, which powers polymorphic transitions between various chiral structures. These findings outline a general strategy for the assembly of reconfigurable chiral materials that can easily be moved, stretched, attached to one another and transformed between multiple conformational states, thus allowing precise assembly and nanosculpting of highly dynamical and designable materials with complex topologies.