碳原子链连接的石墨烯量子点的等离激元激发

基于含时密度泛函理论,研究碳原子链连接的石墨烯纳米结构的等离激元激发和等离激元激发诱导的电子输运。结果表明:随着链的增加,在低能共振区,体系的吸收光谱逐渐红移;当碳原子链较长时,体系在近红外、中红外光谱区都有较强的吸收。在红外光谱区,碳原子链连接的石墨烯纳米结构的等离激元共振模式还取决于碳原子链中原子数的奇偶性;在低能光谱区,强度较大的等离激元共振模式诱导的的电流强度也较大。     

石墨烯量子点二聚物的等离激元激发

基于含时密度泛函理论,研究了石墨烯量子点二聚物的等离激元激发.当2个石墨烯量子点靠近,若量子点间的间隙较大,通过电容性相互作用时,石墨烯量子点二聚物的低能等离激元共振模式随着间隙的减小发生红移.进一步减小间隙时,由于电子的隧穿,二聚物的等离激元共振模式发生了改变,杂化等离激元共振模式形成.杂化等离激元共振模式随着间隙的减小继续红移.石墨烯量子点二聚物等离激元共振模式的演化规律不依赖于石墨烯量子点的形状.     

锑烯纳米结构等离激元的第一性原理研究

利用含时密度泛函理论(time-dependent density functional theory(TDDFT)),研究了锑烯纳米结构表面等离激元的激发特性,并给出了微扰场沿着扶手椅边界和Z字边界激发时锑烯纳米结构的吸收光谱.结果表明沿不同的方向激发,吸收光谱不同.距锑烯纳米结构表面0.9处的能量共振点的电荷密度分布表明,在低能共振区,等离激元共振属于键合二聚体的等离激元模式(BDP).     

石墨烯量子点的等离激元激发

基于含时密度泛函理论,研究石墨烯量子点的等离激元激发。和宏观大小的石墨烯相比,由于量子点的尺寸和量子受限效应,石墨烯量子点的等离激元具有一些不同的特征。在低能共振区,光谱线发生展宽和劈裂。石墨烯量子点的等离激元激发依赖于边界的构型。此外,对称性对于石墨烯量子点的等离激元激发也起着重要的作用。     

线性稠环芳烃连接的石墨烯量子点的等离激元激发

基于含时密度泛函理论,研究线性稠环芳烃连接的石墨烯量子点的等离激元激发.在低能共振区,体系存在2种不同的激发模式.一种激发模式主要位于可见光及近红外光谱区,参与该激发模式的离域化π电子在整个体系中运动;随着线性稠环芳烃链长度的增加,该激发模式发生红移,并且激发强度增大.另一种激发模式主要位于5 e V附近,参与该激发模式的π电子在一个石墨烯量子点中运动,该激发模式基本上不受线性稠环芳烃链长度的影响.此外,线性稠环芳烃连接的石墨烯量子点在近红外光谱区的等离激元激发还依赖于石墨烯量子点的形状.     

基于表面等离激元的量子相干效应的理论研究

起源于金属中自由电子集体振荡的表面等离激元,具有超小的光学模式体积和亚波长局域的近场增益,为纳米尺度上研究光和物质相互作用带来新的机遇．共振的纳米金属结构的近场区域,具有各向异性的珀塞尔系数,并且可以为量子体系提供近场激发．我们理论上演示了基于表面等离激元结构的单分子共振荧光、原子布居数的本征量子拍频及其在表面等离激元结构中的纳米尺度上的实现、表面等离激元诱导的各向异性珀塞尔系数导致的亚波长尺度自发辐射谱线的变化．这些结果在超紧凑的有源量子器件中有潜在应用．     

石墨烯微米带THz SPPs的激发及场分布特性研究

表面等离激元可以突破衍射极限,具有强局域性,在传感、起偏、吸收、分束等方面具有广泛的应用前景.目前,太赫兹波段的表面等离激元器件研究大多是在远场光谱方面,其近场特性的研究有待更进一步深入.本文基于石墨烯微米带结构,研究了太赫兹表面等离激元的激发及场分布特性.本文设计了能够通过太赫兹波激发表面等离激元的石墨烯微米带结构,数值计算了其表面等离激元的场分布,并制备了石墨烯微米带器件,利用透射式太赫兹近场显微镜激发并测量了石墨烯微米带的表面等离激元,对共振失谐对等离激元场分布的影响进行了探究.研究结果为石墨烯表面等离激元器件在太赫兹生物传感、安全检测、高数据率通信等方面的应用提供了相关指导.     

不对称纳米环/椭球二聚体的高阶表面等离激元共振特性

基于三维有限元法,研究了不对称纳米环/椭球二聚体的表面等离激元共振和局域场增强光学特性。结果可得可调的高阶表面等离激元共振,这样的高阶共振源于纳米环和纳米椭球之间的等离激元耦合。同时,在两个纳米结构耦合下,在纳米椭球上可以观察到环形电流,其产生了增强的局域电磁场。数值模拟结果表明,纳米环/椭球二聚体的偏心方向和偏心率对表面等离激元共振有着重要的影响。此结果在表面增强光谱学和生物传感方面都有着潜在的应用。     

基于纳米颗粒阵列与法布里-珀罗干涉结构的超灵敏传感器设计

当前的等离激元传感主要基于表面等离极化激元和局域表面等离激元共振两种模式.然而基于表面等离极化激元的传感需要精确的入射角度及多种光学元器件的配合方能使用;而基于局域表面等离激元共振的传感由于共振线宽较宽导致其灵敏度和品质因数(figure of merit,FOM)不够高.设计了一种基于纳米颗粒/间隔层/反射层结构的具...     

基于石墨烯复合薄膜的等离激元传感研究进展

 做为由单层碳原子紧密堆积而成的六边形蜂窝状二维晶体,石墨烯具有高载流子迁移率、良好的生物兼容性和优异的化学稳定性。本文简要综述了石墨烯-金属纳米粒子复合薄膜在表面增强拉曼散射研究进展,以及石墨烯等离激元的激发方式和传感性能。在可见光波段,石墨烯和金属纳米粒子之间的耦合使复合薄膜具有强的光学吸收和局域电场增强,从而使复合薄膜可以作为高灵敏的表面增强拉曼基底。在中红外波段,除可以利用石墨烯微纳结构激发等离激元,还可以对介电基底进行微纳加工利用波导模式激发,使得石墨烯等离激元可能用于折射率传感。讨论了石墨烯基复合薄膜研究过程中面临的机遇和挑战,展望了其在表面增强拉曼和传感方面的应用前景。     

Optical nano-imaging of gate-tunable graphene plasmons

The ability to manipulate optical fields and the energy flow of light is central to modern information and communication technologies, as well as quantum information processing schemes. However, because photons do not possess charge, a way of controlling them efficiently by electrical means has so far proved elusive. A promising way to achieve electric control of light could be through plasmon polaritons—coupled excitations of photons and charge carriers—in graphene. In this two-dimensional sheet of carbon atoms, it is expected that plasmon polaritons and their associated optical fields can readily be tuned electrically by varying the graphene carrier density. Although evidence of optical graphene plasmon resonances has recently been obtained spectroscopically, no experiments so far have directly resolved propagating plasmons in real space. Here we launch and detect propagating optical plasmons in tapered graphene nanostructures using near-field scattering microscopy with infrared excitation light. We provide real-space images of plasmon fields, and find that the extracted plasmon wavelength is very short—more than 40 times smaller than the wavelength of illumination. We exploit this strong optical field confinement to turn a graphene nanostructure into a tunable resonant plasmonic cavity with extremely small mode volume. The cavity resonance is controlled in situ by gating the graphene, and in particular, complete switching on and off of the plasmon modes is demonstrated, thus paving the way towards graphene-based optical transistors. This successful alliance between nanoelectronics and nano-optics enables the development of active subwavelength-scale optics and a plethora of nano-optoelectronic devices and functionalities, such as tunable metamaterials, nanoscale optical processing, and strongly enhanced light–matter interactions for quantum devices and biosensing applications.     

核/壳型纳米银球的局域表面等离子体共振调谐特性研究

利用离散偶极子理论数值模拟了核/壳结构纳米银球局域表面等离子体共振调谐特性,并应用等离子体杂化理论对其数值结果进行了解释。研究结果表明:对于固定的球壳结构,当改变内核介质的介电常数与内核结构尺寸时,其等离子体共振峰发生了明显的移动现象;对于固定的内核结构,当外核厚度变化时能有效实现共振峰的调控。     

Controlling inelastic light scattering quantum pathways in graphene

Inelastic light scattering spectroscopy has, since its first discovery, been an indispensable tool in physical science for probing elementary excitations, such as phonons, magnons and plasmons in both bulk and nanoscale materials. In the quantum mechanical picture of inelastic light scattering, incident photons first excite a set of intermediate electronic states, which then generate crystal elementary excitations and radiate energy-shifted photons. The intermediate electronic excitations therefore have a crucial role as quantum pathways in inelastic light scattering, and this is exemplified by resonant Raman scattering and Raman interference. The ability to control these excitation pathways can open up new opportunities to probe, manipulate and utilize inelastic light scattering. Here we achieve excitation pathway control in graphene with electrostatic doping. Our study reveals quantum interference between different Raman pathways in graphene: when some of the pathways are blocked, the one-phonon Raman intensity does not diminish, as commonly expected, but increases dramatically. This discovery sheds new light on the understanding of resonance Raman scattering in graphene. In addition, we demonstrate hot-electron luminescence in graphene as the Fermi energy approaches half the laser excitation energy. This hot luminescence, which is another form of inelastic light scattering, results from excited-state relaxation channels that become available only in heavily doped graphene.     

中空银纳米球的制备及其性能研究

新型的金属纳米粒子因为独特的由表面等离子体共振诱导(SPR)的光学性质和很多的潜在应用而受到社会广泛的关注。在具有SPR效应的贵金属纳米粒子中,中空纳米结构有一个很高的散射系数,其共振频率通过改变中空核的尺寸和壳的厚度可以很容易地被控制。本论文中拟采用电化学方法结合电偶置换法在高定向热解石墨(HOPG)及金膜表面制备不同尺寸具有中空结构的银纳米阵列,研究了中空银纳米阵列的局域表面等离子效应(L-SPR),为其在SPR定性和定量研究中的应用提供理论指导。     

金属微纳结构有序阵列中Fano共振的产生条件

本文研究了由椭圆形金纳米颗粒组成的周期阵列在对称介质环境以及放置在介质波导表面两种体系下的Fano共振特性．我们将衍射表面波或波导本征模调谐到金纳米颗粒的局域等离激元共振频率附近,使其满足了通常意义上Fano共振产生的条件,即窄线宽和宽线宽的模式在共振能量上的重叠．我们发现,当仅满足这一条件时,Fano共振并不能被有效激发．我们通过对共振模式场分布的研究分析,阐述了Fano共振的激发还必须满足两种不同线宽的模式需要具有相同的电场分量．我们的研究结果将有助于更好地理解Fano共振的物理意义,对于设计基于Fano共振的微纳光子结构和器件有着重要的指导意义．     

局域表面等离子体增强吸收的超薄太阳能电池的研究

设计了3种不同形状的纳米结构,即圆柱形光栅、长方形光栅、三角形光栅,将其覆盖在硅吸收层表面,利用有限元方法对其进行仿真模拟,结果表明金属光栅激发的局域表面等离子体明显增强了薄膜太阳能电池的吸收效率,通过对比发现圆柱形光栅更能有效地将光能耦合到薄膜硅层中.     

Quantum plasmon resonances of individual metallic nanoparticles

The plasmon resonances of metallic nanoparticles have received considerable attention for their applications in nanophotonics, biology, sensing, spectroscopy and solar energy harvesting. Although thoroughly characterized for spheres larger than ten nanometres in diameter, the plasmonic properties of particles in the quantum size regime have been historically difficult to describe owing to weak optical scattering, metal-ligand interactions, and inhomogeneity in ensemble measurements. Such difficulties have precluded probing and controlling the plasmonic properties of quantum-sized particles in many natural and engineered processes, notably catalysis. Here we investigate the plasmon resonances of individual ligand-free silver nanoparticles using aberration-corrected transmission electron microscope (TEM) imaging and monochromated scanning TEM electron energy-loss spectroscopy (EELS). This technique allows direct correlation between a particle's geometry and its plasmon resonance. As the nanoparticle diameter decreases from 20 nanometres to less than two nanometres, the plasmon resonance shifts to higher energy by 0.5 electronvolts, a substantial deviation from classical predictions. We present an analytical quantum mechanical model that describes this shift due to a change in particle permittivity. Our results highlight the quantum plasmonic properties of small metallic nanospheres, with direct application to understanding and exploiting catalytically active and biologically relevant nanoparticles.     

距离调控纳米多孔金表面增强荧光特性

通过调控纳米多孔金(NPG)基底与荧光分子之间的距离,系统研究了其表面增强荧光特性.利用物理气相沉积方法在NPG表面沉积二氧化硅薄膜,通过调整二氧化硅的厚度来控制NPG与荧光分子之间的距离,系统研究了NPG孔径尺寸以及与荧光分子之间距离对其表面增强荧光(SEF)特性的影响.由于多孔金具有纳米级多孔结构,其表面等离子体能够通过分子附近局域电场的增强使分子的激发光场得到增强,从而提高分子的激发强度和效率;当荧光分子与多孔金表面存在一定距离时,通过与光子之间的共振耦合作用,表面等离子体能够增强多孔金周围电磁场,实现荧光增强.通过研究发现,NPG孔径为36nm、表面二氧化硅厚度为20nm时,表面组装的罗丹明6G荧光分子的荧光强度得到最大增强.     

单层石墨莫比乌斯纳米带的形成判据和能量变化

莫比乌斯带是一种无向的几何面,从带面上任何一点出发都可到达带面上任何一点.可以通过对一个二维矩形带的扭转对接得到莫比乌斯带.单层石墨纳米材料Graphene的发现为研究莫比乌斯带提供了一个真实的物理模型.然而与纯粹几何面不同,在Graphene莫比乌斯带结构中碳原子分布是离散的,由于平面Graphene的平衡键长约为1.42,在形成莫比乌斯带后键长将发生一定变化,这就使得并非对于任意数目的碳原子Graphene平面都会形成相应的莫比乌斯带结构.这里有两个基本问题需要回答：（ⅰ）平面Graphene形成莫比乌斯带需要满足什么条件.（ⅱ）当平面Graphene形成莫比乌斯带之后,由于键长键角的变化引起的能量变化是怎样的.本文第一次系统地研究了这一体系.根据Lindemann判据,我们发现当平面Graphene的横纵单元数之比小于7时,不存在满足我们假设的莫比乌斯带,当Graphene的横纵单元数之比大于50时,存在满足我们假设的莫比乌斯带.当Graphene的横纵单元数之比处于7～50之间时,我们给出了判别莫比乌斯带存在性的计算方法.应用遗传算法我们发现,随着原子数的增加,由平面Graphene变化到莫比乌斯带所产生的弹性形变能是呈指数递减的.