纳米金属微粒的热力学性质研究

电子的分立能级和宇称效应是纳米颗粒的两个重要特征,它们强烈影响纳米金属颗粒的热力学性质.根据随机矩阵理论,考虑能级统计的影响,基于正则系综计算了具有奇数或偶数个电子的纳米金属颗粒的比热和自旋磁化率,并讨论了二者随温度、粒径和电子体密度的变化关系.     

金属纳米颗粒的极化率与异常光学性质

基于金属纳米材料的异常光学现象,考虑了束缚电荷作用的情况,从理论上推导出在光波照射下金属纳米颗粒的极化率与颗粒尺度关系的结果,进而得到金属颗粒对光波的吸收率,并讨论颗粒尺度对极化率和吸收率的影响,即当金属粒子尺寸达到纳米级时,将金属粒子看作纳米小球,小球极化率出现半径的立方因子,且小球半径小于电子平均自由程,电子的衰减因子受小球半径的制约.由推导结果可以得出,光吸收峰增强,并产生红移.这些结果为深入理解金属纳米颗粒的异常光学性质,揭示和开发应用金属纳米材料的性质提供理论基础.     

被囚禁的电子和未来的电子学器件

把自由运动的电子囚禁在一个小的纳米颗粒内,或者在一根非常细的短金属线内,线的宽度只有几个纳米,会发生十分奇妙的事情。由于颗粒内的电子运动受到限制,电子动或能量被量子化了。结果表现在当在金属颗粒的两端加上电压,电压合适时,金属颗粒导电而电压不合适时金属颗粒不导电。这样一来,原本在宏观世界内奉为经典的欧姆定律在纳米世界内不再成立了。还有一种奇怪的现象,当金属纳米颗粒从外电路得到一个额外的电子时,金属颗粒具有了负电性,它的库仑力,足以排斥下一个电子从外电路进入金属颗粒内,切断了电流的连续性,也使得人们想到是否可以发展用一个电子来控制的电子器件,所谓单电子器件。单电子器件的尺寸很小,一旦实现,并把它们集成起来作成计算机芯片。计算机的容量和计算速度不知要提高多少倍。然而,事情可不是像人们所设想的那么简单。起码有两个方面的问题向当前的科学技术     

磁场对超导纳米粒子电子热容的影响

采用随机矩阵理论,考虑能级分离、系统电子总自旋和平均能级间距及转变温度对电子热容的影响,用静态路径近似(SPA)计算了高斯系综中正交系综(GOE)、辛系综(GSE)所对应的电子能级分布下处于弱磁场中超导纳米粒子的电子热容.计算中取了几个典型的温度和电子自旋,并对计算结果做了分析.     

金属纳米颗粒增强太阳能电池光吸收效应研究

采用Mie理论,对球形纳米金属颗粒进行数值计算,研究了金属纳米颗粒在发生表面等离激元共振时表现出的散射效应.改变金属材料类型或者颗粒尺寸大小,金属纳米球的散射效率均发生不同程度的变化.这一现象表明:金属纳米颗粒的散射效应受材料类型和尺寸大小的影响显著.计算结果表明,半径为100nm的Ag纳米颗粒在发生表面等离激元共振时,散射效率最高,吸收效应最弱.     

微波热分解法制备溶剂稳定的钯金属纳米颗粒

首次报道了在丁醇及氢氧化钠条件下,采用微波热分解法加热分解乙酸钯制备了金属钯纳米颗粒,并用TEM、XPS对其进行了表征.结果表明:随着乙酸钯浓度的增加,金属钯纳米颗粒的平均粒径由30 nm增至50 nm.讨论了当乙酸钯浓度为0.5×10-3 mol/L时,氢氧化钠浓度对金属钯纳米颗粒大小的影响.     

精确尺寸巯基保护贵金属纳米团簇的合成进展

金属纳米团簇作为凝聚态物质的初始形态之一,在金属原子/分子化合物向金属纳米颗粒形成的过程中起着桥梁作用.因其具有量子局限效应,团簇往往表现出特异的光学、催化等性质.近几十年来的研究发现,单个原子的改变会对团簇的几何结构以及电子结构产生显著的影响.同时,精确的结构可以有效地建立结构与性质之间的关系.因此,合成具有精确结构的纳米团簇在近年来受到广泛关注.笔者对巯基保护精确结构金属纳米团簇合成方法的建立以及发展进行了综述.     

晶界处碳含量对超纳米金刚石的结构及电学性质影响的第一性原理计算

采用MedeA.软件中基于密度泛函理论(DFT)下的平面波赝势方法的VASP软件包进行模拟,计算了不同晶界处碳含量对超纳米金刚石电子特性和结构特性的影响。从对优化后的结构分析来看,晶界处碳含量的增加会增加超纳米金刚石中sp~2-C的含量,并且会使金刚石晶粒最外层的原子产生一定程度的位移或改变其键角。分析不同晶界处碳含量超纳米金刚石的能带发现,晶界碳含量的增加会减小结构的带隙,并且会在带隙里引入悬键能级和与sp~2-C相关的π*能级。对3个结构态密度的分析发现,晶界含量的增加不仅会减小结构的带隙,还会增加带隙里悬键能级和π*能级的能态密度,减小电子从低能级跃迁到高能级所需的能量,从而增加超纳米金刚石的导电性。     

Ag纳米颗粒修饰TiO2阵列薄膜的制备及其气敏性能研究

以钛酸丁酯为钛源,用水热法在透明导电衬底FTO上制备金红石相TiO2纳米阵列薄膜,以AgNO3为银源,用化学还原法制备尺寸可控的金属Ag纳米颗粒,将所制备的金属Ag颗粒修饰TiO2纳米阵列薄膜.研究Ag纳米颗粒的表面修饰对TiO2纳米阵列薄膜气敏性能的影响.实验结果表明,室温下,18nm金属Ag纳米颗粒修饰后的薄膜对氢气的灵敏度增加,响应和恢复时间减小,气敏性能明显优越于修饰前的薄膜.     

电子气体的宏观特性与维度的关系

本文以金属中的电子气体为例,把金属中的电子气体视为高度简并的费米气体,应用费米-狄拉克分布,从分析电子气体的能量状态出发,导出了电子气体的能级密度,费米能级和化学势;对金属中一至三维电子气体的比热、泡利顺磁性、朗道逆磁性及传导特性进行了较详细的讨论,总结出了电子气体的比热、磁化率、电导、热导及洛伦兹数的计算通式;找出了维度对这些性质的影响.     

能级统计与纳米金属小粒子的磁化率

作者考虑到纳米金属小粒子电子能级分离的特点以及电子数奇偶性的影响，采用能级统计的方法在正则系综中数值计算了纳米金属小粒子的磁化率，并对其在高低温时的特点作了讨论．     

用随机矩阵理论研究常规超导纳米粒子的电子热容

考虑了奇/偶电子数分布,用静态路径近似(SPA)方法计算了随机矩阵理论中高斯正交系综(GOE)所对应的电子能级分布下常规超导纳米粒子的电子热容,得到了弱自旋轨道耦合和弱磁场中奇/偶电子数分布下相变临界区域附近的电子热容,并做了简单分析.     

纳米量级超导粒子电子比热中的量子尺寸效应

考虑了奇/偶电子数分布,从配分函数出发,用静态路径近似(SPA)方法和BCS方法计算了随机矩阵理论中高斯正交系综(GOE)所对应的电子能级分布对超导纳米粒子的电子比热的影响,得到了弱自旋-轨道耦合和弱磁场中和奇/偶电子数分布下的电子比热,并做了简单分析.经过计算和分析,发现粒子尺寸和奇/偶电子数对电子比热和转变温度有影响.     

超导金属小粒子的电子比热研究

利用随机矩阵理论中能级统计的方法,考虑能级分布和能级关联的影响,给出适合于金属小粒子的自恰方程,并详细数值计算了无外场作用时超导金属小粒子s=0及s=1/2两个自旋态能隙参量和临界转变温度随金属小粒子粒径的变化规律,以及在不同粒径时的电子比热.并在自旋s=0时理论结果得到了实验上观察到的超导增强效应.     

强耦合多电子相互作用比热

在强耦合极限和任意电子密度下,得到了多电子相互作用比热与温度和电子密度间的解析形式。讨论了多电子相互作用参量对比热的影响。与数字解比较,解析解便于分析,且适用温度范围加宽了。     

Electrical detection of spin precession in a metallic mesoscopic spin valve

To study and control the behaviour of the spins of electrons that are moving through a metal or semiconductor is an outstanding challenge in the field of 'spintronics', where possibilities for new electronic applications based on the spin degree of freedom are currently being explored. Recently, electrical control of spin coherence and coherent spin precession during transport was studied by optical techniques in semiconductors. Here we report controlled spin precession of electrically injected and detected electrons in a diffusive metallic conductor, using tunnel barriers in combination with metallic ferromagnetic electrodes as spin injector and detector. The output voltage of our device is sensitive to the spin degree of freedom only, and its sign can be switched from positive to negative, depending on the relative magnetization of the ferromagnetic electrodes. We show that the spin direction can be controlled by inducing a coherent spin precession caused by an applied perpendicular magnetic field. By inducing an average precession angle of 180 degrees, we are able to reverse the sign of the output voltage.     

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.     

Room-temperature ferromagnetic nanotubes controlled by electron or hole doping

Nanotubes and nanowires with both elemental (carbon or silicon) and multi-element compositions (such as compound semiconductors or oxides), and exhibiting electronic properties ranging from metallic to semiconducting, are being extensively investigated for use in device structures designed to control electron charge. However, another important degree of freedom--electron spin, the control of which underlies the operation of 'spintronic' devices--has been much less explored. This is probably due to the relative paucity of nanometre-scale ferromagnetic building blocks (in which electron spins are naturally aligned) from which spin-polarized electrons can be injected. Here we describe nanotubes of vanadium oxide (VO(x)), formed by controllable self-assembly, that are ferromagnetic at room temperature. The as-formed nanotubes are transformed from spin-frustrated semiconductors to ferromagnets by doping with either electrons or holes, potentially offering a route to spin control in nanotube-based heterostructures.     

Thermal spin current from a ferromagnet to silicon by Seebeck spin tunnelling

Heat generation by electric current, which is ubiquitous in electronic devices and circuits, raises energy consumption and will become increasingly problematic in future generations of high-density electronics. The control and re-use of heat are therefore important topics for existing and emerging technologies, including spintronics. Recently it was reported that heat flow within a ferromagnet can produce a flow of spin angular momentum-a spin current-and an associated voltage. This spin Seebeck effect has been observed in metallic, insulating and semiconductor ferromagnets with temperature gradients across them. Here we describe and report the demonstration of Seebeck spin tunnelling-a distinctly different thermal spin flow, of purely interfacial nature-generated in a tunnel contact between electrodes of different temperatures when at least one of the electrodes is a ferromagnet. The Seebeck spin current is governed by the energy derivative of the tunnel spin polarization. By exploiting this in ferromagnet-oxide-silicon tunnel junctions, we observe thermal transfer of spins from the ferromagnet to the silicon without a net tunnel charge current. The induced spin accumulation scales linearly with heating power and changes sign when the temperature differential is reversed. This thermal spin current can be used by itself, or in combination with electrical spin injection, to increase device efficiency. The results highlight the engineering of heat transport in spintronic devices and facilitate the functional use of heat.     

Half-metallic graphene nanoribbons

Electrical current can be completely spin polarized in a class of materials known as half-metals, as a result of the coexistence of metallic nature for electrons with one spin orientation and insulating nature for electrons with the other. Such asymmetric electronic states for the different spins have been predicted for some ferromagnetic metals--for example, the Heusler compounds--and were first observed in a manganese perovskite. In view of the potential for use of this property in realizing spin-based electronics, substantial efforts have been made to search for half-metallic materials. However, organic materials have hardly been investigated in this context even though carbon-based nanostructures hold significant promise for future electronic devices. Here we predict half-metallicity in nanometre-scale graphene ribbons by using first-principles calculations. We show that this phenomenon is realizable if in-plane homogeneous electric fields are applied across the zigzag-shaped edges of the graphene nanoribbons, and that their magnetic properties can be controlled by the external electric fields. The results are not only of scientific interest in the interplay between electric fields and electronic spin degree of freedom in solids but may also open a new path to explore spintronics at the nanometre scale, based on graphene.