Breakdown of Fermi-liquid theory in a copper-oxide superconductor.

The behaviour of electrons in solids is well described by Landau's Fermi-liquid theory, which predicts that although electrons in a metal interact, they can still be treated as well defined fermions, which are called 'quasiparticles'. At low temperatures, the ability of quasiparticles to transport heat is given strictly by their ability to transport charge, as described by a universal relation known as the Wiedemann-Franz law, which hitherto no material has been known to violate. High-temperature superconductors have long been thought to fall outside the realm of Fermi-liquid theory, as suggested by several anomalous properties, but this has yet to be shown conclusively. Here we report an experimental test of the Wiedemann-Franz law in the normal state of a copper-oxide superconductor, (Pr,Ce)2CuO4, which reveals that the elementary excitations that carry heat in this material are not fermions. This is compelling evidence for the breakdown of Fermi-liquid theory in high-temperature superconductors.     

Determination of electron orbital magnetic moments in carbon nanotubes

The remarkable transport properties of carbon nanotubes (CNTs) are determined by their unusual electronic structure. The electronic states of a carbon nanotube form one-dimensional electron and hole sub-bands, which, in general, are separated by an energy gap. States near the energy gap are predicted to have an orbital magnetic moment, mu(orb), that is much larger than the Bohr magneton (the magnetic moment of an electron due to its spin). This large moment is due to the motion of electrons around the circumference of the nanotube, and is thought to play a role in the magnetic susceptibility of CNTs and the magnetoresistance observed in large multiwalled CNTs. But the coupling between magnetic field and the electronic states of individual nanotubes remains to be quantified experimentally. Here we report electrical measurements of relatively small diameter (2-5 nm) individual CNTs in the presence of an axial magnetic field. We observe field-induced energy shifts of electronic states and the associated changes in sub-band structure, which enable us to confirm quantitatively the predicted values for mu(orb).     

High-resolution spectroscopy of two-dimensional electron systems

Spectroscopic methods involving the sudden injection or ejection of electrons in materials are a powerful probe of electronic structure and interactions. These techniques, such as photoemission and tunnelling, yield measurements of the 'single-particle' density of states spectrum of a system. This density of states is proportional to the probability of successfully injecting or ejecting an electron in these experiments. It is equal to the number of electronic states in the system able to accept an injected electron as a function of its energy, and is among the most fundamental and directly calculable quantities in theories of highly interacting systems. However, the two-dimensional electron system (2DES), host to remarkable correlated electron states such as the fractional quantum Hall effect, has proved difficult to probe spectroscopically. Here we present an improved version of time-domain capacitance spectroscopy that allows us to measure the single-particle density of states of a 2DES with unprecedented fidelity and resolution. Using the method, we perform measurements of a cold 2DES, providing direct measurements of interesting correlated electronic effects at energies that are difficult to reach with other techniques; these effects include the single-particle exchange-enhanced spin gap, single-particle lifetimes in the quantum Hall system, and exchange splitting of Landau levels not at the Fermi surface.     

一维无序系统电子结构

本文应用负本征值理论方法,计算了含有上万个粒子的一维无序系统的电子态密度,针对无序程度和系统大小等物理量,讨论了无序系统的电子结构。结果表明,随着无序程度的变大,电子的局域化程度加强,而随着无序系统的变大,局域化的电子数增多。     

Evidence for spin-charge separation in quasi-one-dimensional organic conductors

Interacting conduction electrons are usually described within Fermi-liquid theory, which states that, in spite of strong interactions, the low-energy excitations are electron-like quasiparticles with charge and spin. In recent years there has been tremendous interest in conducting systems that are not Fermi liquids, motivated by the observation of highly anomalous metallic states in various materials, most notably the copper oxide superconductors. Non-Fermi-liquid behaviour is generic to one-dimensional interacting electron systems, which are predicted to be Luttinger liquids. One of their key properties is spin-charge separation: instead of quasiparticles, collective excitations of charge (with no spin) and spin (with no charge) are formed, which move independently and at different velocities. However, experimental confirmation of spin-charge separation remains a challenge. Here we report experiments probing the charge and heat current in quasi-one-dimensional conductors--the organic Bechgaard salts. It was found that the charge and spin excitations have distinctly different thermal conductivities, which gives strong evidence for spin-charge separation. The spin excitations have a much larger thermal conductivity than the charge excitations, which indicates that the coupling of the charge excitations to the lattice is important.     

How Cooper pairs vanish approaching the Mott insulator in Bi2Sr2CaCu2O8+delta

The antiferromagnetic ground state of copper oxide Mott insulators is achieved by localizing an electron at each copper atom in real space (r-space). Removing a small fraction of these electrons (hole doping) transforms this system into a superconducting fluid of delocalized Cooper pairs in momentum space (k-space). During this transformation, two distinctive classes of electronic excitations appear. At high energies, the mysterious 'pseudogap' excitations are found, whereas, at lower energies, Bogoliubov quasi-particles-the excitations resulting from the breaking of Cooper pairs-should exist. To explore this transformation, and to identify the two excitation types, we have imaged the electronic structure of Bi(2)Sr(2)CaCu(2)O(8+delta) in r-space and k-space simultaneously. We find that although the low-energy excitations are indeed Bogoliubov quasi-particles, they occupy only a restricted region of k-space that shrinks rapidly with diminishing hole density. Concomitantly, spectral weight is transferred to higher energy r-space states that lack the characteristics of excitations from delocalized Cooper pairs. Instead, these states break translational and rotational symmetries locally at the atomic scale in an energy-independent way. We demonstrate that these unusual r-space excitations are, in fact, the pseudogap states. Thus, as the Mott insulating state is approached by decreasing the hole density, the delocalized Cooper pairs vanish from k-space, to be replaced by locally translational- and rotational-symmetry-breaking pseudogap states in r-space.     

氮铝簇合物的结构与稳定性

采用密度泛函理论（DFT）中的B3LYP方法,以6－31G标准基组加一个极化函数,对（ClAlNH)10和（AlN)10簇合物分子的几何构型、电子结构和红外光谱进行了优化计算,并讨论了它们的化学键特征。研究结果表明,（ClAlNH)10和（AlN)10簇合物的基态稳定结构均具有C2h对称,不存在Al-Al和N－N键,因此Al-N键是惟一的键型。     

CsI高压超导电性的第一性原理

利用基于密度泛函理论的赝势平面波方法计算了高压下CsI的电子能带结构、 电子态密度、 声子谱、 声子态密度以及电子和声子的相互作用, 探讨了CsI在高压下产生超导电性的物理机制. 研究表明, CsI层内的光学振动模式与电子之间的强耦合作用是CsI产生超导电性的主要原因.     

Emerging local Kondo screening and spatial coherence in the heavy-fermion metal YbRh2Si2

The entanglement of quantum states is both a central concept in fundamental physics and a potential tool for realizing advanced materials and applications. The quantum superpositions underlying entanglement are at the heart of the intricate interplay of localized spin states and itinerant electronic states that gives rise to the Kondo effect in certain dilute magnetic alloys. In systems where the density of localized spin states is sufficiently high, they can no longer be treated as non-interacting; if they form a dense periodic array, a Kondo lattice may be established. Such a Kondo lattice gives rise to the emergence of charge carriers with enhanced effective masses, but the precise nature of the coherent Kondo state responsible for the generation of these heavy fermions remains highly debated. Here we use atomic-resolution tunnelling spectroscopy to investigate the low-energy excitations of a generic Kondo lattice system, YbRh(2)Si(2). We find that the hybridization of the conduction electrons with the localized 4f electrons results in a decrease in the tunnelling conductance at the Fermi energy. In addition, we observe unambiguously the crystal-field excitations of the Yb(3+) ions. A strongly temperature-dependent peak in the tunnelling conductance is attributed to the Fano resonance resulting from tunnelling into the coherent heavy-fermion states that emerge at low temperature. Taken together, these features reveal how quantum coherence develops in heavy 4f-electron Kondo lattices. Our results demonstrate the efficiency of real-space electronic structure imaging for the investigation of strong electronic correlations, specifically with respect to coherence phenomena, phase coexistence and quantum criticality.     

基于分子轨道特征苏氨酸分子体系的电子激发类型

基于优化的右旋苏氨酸（R-Thr）分子结构, 在PBE0/def2-TZVP下, 用含时密度泛函理论（TDDFT）方法得到气相条件、 隐式H₂O和甲醇溶剂环境下R-Thr分子体系电子激发过程中激发态波函数的计算结果, 并通过指认分子轨道类型方法研究R-Thr分子体系价层电子的激发类型. 结果表明： 隐式溶剂环境比气相环境更适合研究R-Thr分子体系的电子激发特性; 分子轨道（MO）类型与Δr指数分析结果较理想, 大部分激发态的激发类型与激发模式指认吻合度较高.     

基于分子轨道特征苏氨酸分子体系的电子激发类型

基于优化的右旋苏氨酸（R-Thr）分子结构, 在PBE0/def2-TZVP下, 用含时密度泛函理论（TDDFT）方法得到气相条件、 隐式H₂O和甲醇溶剂环境下R-Thr分子体系电子激发过程中激发态波函数的计算结果, 并通过指认分子轨道类型方法研究R-Thr分子体系价层电子的激发类型. 结果表明： 隐式溶剂环境比气相环境更适合研究R-Thr分子体系的电子激发特性; 分子轨道（MO）类型与Δr指数分析结果较理想, 大部分激发态的激发类型与激发模式指认吻合度较高.     

不同氧化锆相的稳定性及电子结构的第一性原理研究

通过密度泛函理论计算了不同氧化锆相的晶体结构参数,在所有晶相模型结构优化的基础上,分析了在一般温度和压力下不同晶相稳定程度不同的原因。使用3种不同的泛函计算了不同晶相的电子能带结构和态密度电荷差分密度,发现在氧化锆高温稳定相体系中,由于强关联电子的相互作用增强,传统密度泛函理论的广义梯度近似平面波超软赝势泛函及其修正的Hubbard U方法都会严重低估能带带隙,因此所得各层能带位置不准确,而使用B3LYP杂化泛函计算的结果则可以很好地与已有实验结果相吻合。结合杂化泛函计算出的态密度和差分密度数据,在理论上从电子间相互作用的角度解释了氧化锆不同晶相的稳定性、导电性及光吸收性能。     

单体苏氨酸分子和离子体系的激发态特性

采用密度泛函理论(DFT)中的B3LYP方法, 在6-311+G(2-df)基组水平上优化单体苏氨酸(Thr)分子和离子体系的基态稳定几何构型, 并用含时密度泛函理论(TD-DFT)方法研究隐式溶剂乙醇下单体Thr分子和离子体系各激发态的特性. 结果表明： 随着分子捕获电子数目的增加, 体系的能带 略减小； 单体Thr^2-体系的S1~S10激发态均由占据轨道MO33得到； 该体系的Rydberg激发特性较好, 捕获电子离子体系的激发态激发模式发生了显著变化.     

Ti原子位置对立方SrTiO3电子结构的影响

基于第一性原理密度泛函理论框架下的平面波超软赝势计算方法,计算分析了Ti原子Z轴分数坐标的移动对立方SrTiO 3的能带结构、能态密度和Mulliken电荷布居方面的电子结构的影响。计算结果表明,随着Ti原子Z坐标的上移,O原子的电子逐渐转移到Ti原子上,使得O的部分电子能量升高,Ti的部分电子能量降低,价带与导带渐渐重叠,能隙消失,即Ti原子位置可以强烈影响SrTiO 3的电子结构。     

基于密度泛函理论和含时密度泛函理论下富勒烯B24N24光谱性质研究

本文在B3LYP/6-31g(d)基组水平上, 利用密度泛函理论(DFT)优化了B24N24团簇的几何和电子结构. 研究结果表明, 优化所得B24N24团簇的几何结构对称性分别为S4、C2、S8和O;在基态稳定结构基础上, 得出其输运性质, 既非p型输运材料, 亦非n型输运材料, 即不具有输运性质;在优化好的基态结构基础上, 又研究了它的红外和拉曼分子振动谱, 四种团簇的红外-拉曼振动谱的振动强度排序均为O>S8>S4>C2;随后采用含时密度泛函理论(TDDFT),同样在B3LYP/6-31g(d)基组水平上, 计算了这四种物质在CH2Cl2溶剂中的UV-Vis吸收谱特性, 研究表明跃迁能级数量越多,吸收谱振动强度越强, 并且这些分子的紫外-可见吸收谱的振动强度排序为S4>C2>S8>O.     

分子链长对分子结电输运性质的影响

利用杂化密度泛函理论,研究了烷烃硫醇分子与金电极形成分子结的电子结构,利用弹性散射格林函数方法研究了烷烃硫醇分子的电输运性质,并同实验结果进行了比较。研究结果表明,在低的外加偏压下,烷烃硫醇分子电流值随着分子链长度的增加而指数减小。     

钨酸钡电子结构的第一性原理研究

通过基于密度泛函理论(DFT)框架下广义梯度近似平面波超软赝势法,优化了晶胞的几何结构,计算了白钨矿结构的BaWO4基态的能带结构和电子结构;研究发现:BaWO4为直接带隙结构,带隙宽带为4.5 eV,费米面处的价带主要由W5p和O2p态上电子构成,导带主要是W5d和O2p;根据晶体场理论和分子轨道理论分析了钨酸钡晶体的分子轨道成键,其结果与计算得到的态密度图能较好吻合。关键词:     

气相环境Ala分子和离子的低激发态性质

用密度泛函理论中的B3LYP方法, 在6-311++G(-d,p-)基组水平上, 优化得到气相环境丙氨酸分子和带电离子的基态稳定构型, 并用含时密度泛函理论（TD-DFT)方法研究气相环境丙氨酸分子和负离子的低激发态特性. 结果表明, 随着体系分子获得电子数的增加, 键长呈逐渐减小趋势, 第一激发态的激发能Δ E明显减小, 荧光波长急剧增加, S6电子跃迁轨道数增加.