Na原子链表面等离激元特性的含时密度泛函研究

本文用含时密度泛函理论研究了线性Na原子链的表面等离激元机理.主要在原子尺度下模拟计算了体系随着原子数增加及原子间距变化的集体激发过程.研究发现线性原子链有一个普遍的特性——存在一个纵模和两个横模.两个横模一般在实验上很难被观测到.纵模随着原子链长度增加,能量红移的同时,该纵模主峰的强度呈线性增长.随着原子个数的增加,端点模式(TE)开始蓝移,能量和偶极强度都逐渐趋向饱和.横模能量被劈裂的原因概括如下:(一)每个位置的电子受到的势不同,在两端的电子受到的势要比在中间的电子受到的势要高,因此两端的电荷积累也比中间多;(二)端点存在悬挂键,所以中间的电子-电子间相互作用与端点的不一样,这两方面又都与原子间距d有关.     

介观尺寸原子链中的等离激元：紧束缚模型

本文运用紧束缚模型对介观尺寸原子链的等离激发进行了系统的研究, 通过量子响 应理论和相无规近似得到了等离激元的本征频率方程, 通过该方程计算了系统中等离子体的激发能量, 并分别对体系的本征振荡以及外电场作用在原子链上发生共振的情况进行了研究. 结果表明, 体系在外场作用下发生共振时, 偶极矩的峰值与等离子体的激发态相对应, 说明外场此时激发了等离激元; 体系处在共振情况下, 电荷振荡的幅度远远大于非共振的情况, 相对来说体系的电荷虚部的共振更为明显. 对于体系的本征等离振荡频率, 同等长度时等离子体的激发能量总是大于同级的单电子激发能量; 等离激元的能谱与原子链的长度和电子密度以及系统的库仑关联强度都有很大关系; 在原子链长度保持不变的情况下, 等离子体的激发能量随电子数目的变化以半满为中心呈对称关系. 关键词： 纳米结构 一维原子链 等离激元     

Experimental measurement of acoustic plasmons in polycrystalline palladium

An experimental study of collective oscillations in Pd covering the region of very low energy and momentum transfers is reported. Through Dynamic Electron Scattering spectroscopy, structure factor spectra were measured from 80?K to 298?K on a bulk polycrystalline Pd sample. Here we report the first experimental evidence of damped acoustic plasmons and their evolution to the single-particle excitation continuum. The acoustic plasmons follow a linear dispersion and are experimentally shown to be a separate and distinct resonance mode from acoustic surface plasmons. Calculations of the dielectric function employed a model that incorporates complete mixing of two conduction bands with contributions from both interband and intraband transitions. The model was used in computational studies that focused on specific experimental results to aid the characterization and understanding of the plasmon behavior. We found that the Pd acoustic plasmon energy matched the longitudinal phonon anomaly that has sparked numerous theoretical reports on the possible energetic coupling of these modes. Further experimental evidence of plasmon and phonon dynamical processes are found in the linewidth analysis of the data. The primary decay mechanism of the plasmons is interpreted to be strong phonon-assisted interband transitions. Further spectral features and the plasmon velocity are also reported.     

Slowing light in diatomic nanoshelled chains

Coupled plasmon modes have been studied theoretically in periodic chains of shelled and unshelled metal nanoparticles embedded alternatively in a dielectric host, thus forming a diatomic chain. We calculate the dispersion relation of the diatomic chains and show that we can tune the shelled particle band into the unshelled particle band by varying the permittivity contrast and/or the core-shell radius ratio. This offers a precise control of the group velocity of coupled plasmon modes. The experimental realization of such diatomic chains by surface plasmon enhanced binding will be discussed.     

周期地嵌入电介质球壳的金属表层的表面等离子激元及其与电介质腔体模式的耦合

通过观察金属底板中周期地嵌入电介质球壳的体系的光学吸收性质，研究了表面等离子激元 以及与其他电磁模式的耦合特性.在这种周期结构的金属表面，发现存在两种响应频率，分 别对应于表面等离子激元模式和金属中的电介质腔体模式.在这些响应频率上，可观察到与 它们相对应的吸收峰.由于金属的表面模式不能与平面入射光直接耦合，而腔体模式与平面 入射光和表面等离子激元模式的耦合一般较弱，因而通常情况下这些吸收峰的峰值有限.然 而，通过调整体系中的某些参数，可以使腔体模式和表面模式的频率非常接近，这时二者之 间的耦合强度将大大提高.此时，在相应的频率附近可观察到极强的吸收峰.详细地研究了介 质球壳的物理和几何参数对此共振吸收的影响. 关键词： 腔体模式 表面等离子体模式 共振吸收     

二维方形量子点体系等离激元的量子化

量子点体系等离激元的研究是光电子学领域的热点.为进一步加深和完善对等离激元的量子效应的认识,本文利用紧束缚近似和线性响应理论研究了二维方形量子点体系对外场的集体响应.结果表明,当外场频率等于等离激元的频率时,量子点体系会有强烈的电荷振荡,并伴随着能量的极大吸收和近场的增强.在量子点中,等离子体存在分立的元激发.等离子体元激发的个数将随着量子点尺寸和电子个数的增加而增加.随量子点尺寸的增加,分立的等离激元将逐步呈现准连续的特性,即过渡为经典连续的等离激元,其频谱曲线演化为经典的色散曲线.结果还表明:随量子点尺寸的增加,等离激元的频率会红移,等离激元的激发强度会增大;随量子点中电子数的增加,等离激元的频率会蓝移,等离激元的激发强度会增大.     

Deviating from the nanorod shape: Shape-dependent plasmonic properties of silver nanorice and nanocarrot structures

Noble metallic nanostructures exhibit special optical properties resulting from excitation of surface plasmons. Among the various metallic nanostructures, nanorods have attracted particular attention because of their unique and intriguing shape-dependent plasmonic properties. Nanorods can support transverse and longitudinal plasmon modes, the latter ones depending strongly on the aspect ratio of the nanorod. These modes can be routinely tuned from the visible to the near-infrared spectral regions. Although nanorods have been investigated extensively, there are few studies devoted to nanostructures deviating from the nanorod shape. This review provides an overview of recent progress in the development of two kinds of novel quasi-one-dimensional silver nanostructures, nanorice and nanocarrot, including their syntheses, crystalline characterizations, plasmonic property analyses, and performance in plasmonic sensing applications.     

Effect of transition metal (Fe, Cu, Ni, Rh)-doped small silver chains on optics of plasmon resonances

Doping can control and tune the optical properties of current nanoalloys. In this study, the optical generation of plasmon resonance mode in pure-Ag and transition metal (Fe, Cu, Ni, Rh) single-doped Ag chains is investigated using time-dependent density functional theory. Results show that the redshift of plasmon energy appears and intensity of longitudinal mode enhances with increasing the number of Ag atoms in pure silver chains. The Ag chains doped with transition metal (TM) atom create an additional peak with a local plasmon resonance mode which is related to charge redistribution in the chain around TM atom.     

Collective mode dispersions of organic chain compounds

We investigate the collective mode dispersions for the tight-binding dielectric matrix with two one-dimensional electron bands per donor and acceptor chains, and the three-dimensional long-range Coulomb electron-electron interaction within the random phase approximation. The hybridized collective modes are the result of the strong coupling between the intraband plasmon and the interband dipolar modes due to strong dipole Coulomb interactions. Our calculations show the existence of the low-energy renormalized plasmon mode above the electron-hole quasi-continuum in the long wavelength limit. The obtained modes are brought into correspondence with the optical data of quasi-one-dimensional organic conductor tetrathiafulvalene-tetracyanoquinodimethane (TTF-TCNQ). Namely, the renormalized plasmon and the dipolar mode are assigned to the observed excitations at respective energy scales of roughly 10 meV and 0.75 eV, explaining why lower excitation is eliminated while higher excitation persists below the temperature of the Peierls phase transition.     

Anisotropic plasmon dispersion and damping in multilayer 8-Pmmn borophene structures

We investigate the collective plasma oscillations theoretically in multilayer 8-Pmmn borophene structures, where the tilted Dirac electrons in spatially separated layers are coupled via the Coulomb interaction. We calculate the energy dispersions and Landau dampings of the multilayer plasmon excitations as a function of the total number of layers, the interlayer separation, and the different orientations. Like multilayer graphene, the plasmon spectrum in multilayer borophene consists of one in-phase optical mode and N - 1 out-of-phase acoustical modes. We show that the plasmon modes possess kinks at the boundary of the interband single-particle continuum and the apparent anisotropic behavior. All the plasmon modes approach the same dispersion at a sufficiently large interlayer spacing in the short-wavelength limit. Especially along specific orientations, the optical mode could touch an energy maximum in the nondamping region, which shows non-monotonous behavior. Our work provides an understanding of the multilayer borophene plasmon and may pave the way for multilayer borophene-based plasmonic devices.     

Energy-loss function of TTF-TCNQ

We investigate the energy-loss function for a previously developed model of quasi-one-dimensional metals with two one-dimensional electron bands per donor and acceptor chains and the three-dimensional long-range Coulomb electron-electron interaction within the random phase approximation. It is essentially influenced by two hybridized collective modes which result from the strong coupling of the intraband plasmon and the interband dipolar modes. Our calculations show that the spectral weights of the renormalized plasmon and the dipolar mode dominate within the long wavelength limit, while for large longitudinal wave vectors the intraband electron-hole quasi-continuumgains some experimentally observable spectral weight as the second mode approaches it. The function obtained is brought into correspondence with the data of the quasi-one-dimensional organic conductor tetrathiafulvalene-tetracyanoquinodimethane (TTF-TCNQ) obtained from electron energy-loss spectroscopy (EELS) measurements.     

不同预淀积层银膜表面等离子激元波的辐射效率

测量了棱镜／ＬＢ膜／银膜／空气，棱镜／银膜／空气，棱镜／银膜／空气三种结构在衰减全反射条件下激发的表面等离子激元波由于银膜－空气界面粗糙度而散射以空气中的辐射效率，同时，由散射光强分布计算出表面度粗糙度参数随横向相关长度σ和表面波纹深度δ，再由σ和δ计算出理论辐射效率，理论与实验结果相符合。     

Radiative plasmon polaritons in multilayer structures with a two-dimensional electron gas

Two-dimensional plasmon polaritons are analyzed for a typical experimental configuration in which a layer of two-dimensional electrons with a finite mobility lies on the top of a dielectric waveguide formed by the substrate (a wafer of finite thickness). Two-dimensional plasmons couple strongly to the radiative modes of this dielectric waveguide. It is shown that, as a result of the competition between collisional and radiative processes, a family of eight quasi-stationary normal modes arises. Six of them decay carrying energy to infinity. The two remaining plasmon-polariton modes are nonradiative. One of these modes, the TM-type plasmon polariton, in the limiting case where retardation is disregarded corresponds to the conventional longitudinal two-dimensional plasmon. The other mode, the TE-type plasmon polariton, exists only for a finite thickness of the substrate. All of them are characterized by different dispersion relations of the complex frequency ω(q) = Reω + iImω and differ in both polarization (longitudinal and transverse) and symmetry with respect to the direction of decay (symmetric and asymmetric). The latter modes decay slowly, propagating into free space to plus or minus infinity. The conditions under which the Q factors of certain modes are arbitrarily high are found. In this case, Imω(q ₀) = 0, and dissipative losses in the two-dimensional electron gas are compensated by external sources. As a result, the reflection coefficient for a plane wave whose angle of incidence is determined by the vector q ₀ vanishes.     

Electromagnetic Propagation in a Relativistic Electron Gas at Finite Temperatures

The electromagnetic propagation in a relativistic electron gas at finite temperatures and carrier densities is described. Using quantum electrodynamics at finite temperatures, electric and magnetic responses and general constitutive relations are obtained. Rewriting the propagator for the electromagnetic field in terms of the electric and magnetic responses, the modes that propagate in the gas are identified. As expected, the usual collective excitations are obtained, i.e., a longitudinal electric and two transverse magnetic plasmonic modes. In addition, a purely photonic mode is found, which satisfies the wave equation in vacuum, for which the electron gas is transparent. Dispersion relations for the plasmon modes at zero and finite temperatures are presented and the intervals of frequency and wavelength where both electric and magnetic responses are simultaneously negative are identified, a behavior previously thought not to occur in natural systems. The investigation of the electromagnetic responses of a relativistic electron gas shows that, apart from the usual longitudinal electric plasmon mode and the two transverse magnetic plasmon modes, there is also a pure photonic mode that propagates with the speed of light, as if the medium were transparent. Furthermore, there is a region of frequencies and wavenumbers of the external fields where both the longitudinal electric permittivity and magnetic permeability are simultaneously negative, a property found in artificially constructed metamaterials.     

Surface plasmon resonance and field confinement in graphene nanoribbons in a nanocavity

In this work, we demonstrate surface plasmon resonance properties and field confinement under a strong interaction between a waveguide and graphene nanoribbons (GNRs), obtained by coupling with a nanocavity. The optical transmission of a waveguide–cavity–graphene structure is investigated by finite-difference time-domain simulations and coupled-mode theory. The resonant frequency and intensity of the GNR resonant modes can be precisely controlled by tuning the Fermi energy and carrier mobility of the graphene, respectively. Moreover, the refractive index of the cavity core, the susceptibility χ⁽³⁾ and the intensity of incident light have little effect on the GNR resonant modes, but have good tunability to the cavity resonant mode. The cavity length also has good tunability to the resonant mode of cavity. A strong interaction between the GNR resonant modes and the cavity resonant mode appears at a cavity length of L₁ = 350 nm. We also demonstrate the slow-light effect of this waveguide–cavity–graphene structure and an optical bistability effect in the plasmonic cavity mode by changing the intensity of the incident light. This waveguide–cavity–graphene structure can potentially be utilised to enhance optical confinement in graphene nano-integrated circuits for optical processing applications.     

Influence of amount of CTAB and ascorbic acid concentration on localized surface plasmon resonance property of gold nanorod

Gold nanorods (AuNRs) are prepared through seeded growth approach. Synthesis parameters of the amount of cetyltrimethylammonium bromide (CTAB), and concentration of ascorbic acid (AA) were studied. We were aiming for an aspect ratio of 3 which could be achieved by a nanorod feature in the range of 45 nm length and 15 nm width. The absorption spectra are observed with an UV–visible NIR spectrophotometer and analysed theoretically. It is known that there are two plasmon resonance peaks for gold nanorod corresponding to transverse surface plasmon resonance (TSPR) and longitudinal surface plasmon resonance (LSPR), respectively. It is found that as the concentration of CTAB increases, the yield of NRs increases. As the concentration of AA increased from 0.05 to 0.2 M, LSP shifts to longer wavelength but upon further increasing the concentration, LSP shifts back to shorter wavelength. A linear relationship between LSPR wavelength and surrounding medium dielectric constant is obtained, which is in good agreement with the theoretical results.     

Optical interaction in a plasmonic metallic particle chain coupled to a metallic film

We study the coupling of localized surface plasmon and surface plasmon polariton modes in a system composed of a metallic nanoparticle chain imbedded in a dielectric–metal–dielectric substrate. The results show the influence of outside parts and imbedded parts of particles on the interaction between localized surface plasmon and surface plasmon polariton modes. An enhancement can be observed in our structure. This kind of the structure has a very promising candidate for biosensing and surface enhanced spectroscopy applications.     

Zeeman双频激光器频率分裂与纵模间隔变动一致性分析

激光谐振腔内相位各向异性会引起频率分裂,两分裂模的频差大小由表现出的相位延迟所决定.对于腔内相位延迟较小的He-Ne激光器,两分裂模很接近,处于烧孔重叠区,存在模式竞争而不能同时振荡,形成隐频率分裂.同时,使得激光器两正交偏振方向上的相邻级纵模产生固定的变动量,其大小等于隐频率分裂量的2倍.如果沿激光偏振方向施加横向磁场,Ne原子谱线发生横向Zeeman分裂,增益原子分成两群,分别为平行于磁场和垂直于磁场方向偏振的光提供增益,大大减弱模竞争,使得激光器的两分裂模可同时振荡并测得频差.在谐振腔内放入倾斜的石英晶体片或半波片,由两种方法分别测量频率分裂量并进行比较.实验表明两种方法测量的结果均与理论计算相符,平均相对偏差不超过1%.据此可以准确得到Zeeman双频激光器的频差大小,并为半波片测量提供了新方法.     

A computational study of the optical response of strongly coupled metal nanoparticle chains

We study the optical response of strongly coupled metal nanoparticle chains using rigorous multiple scattering calculations. The collective resonant frequency of silver nanosphere chains and the coupling between chains are considered. The coupling between silver nanoparticle chains are understood by the transmission and reflection calculations of 2D periodic arrays of nanospheres. The results are in agreement with recent experiments. The splitting of plasmon resonance modes for different polarizations of the incident light are explored. Our results show that the transverse mode resonant wavelength is very sensitive to the inter-chain distance. Results on the effect of disorder are also presented.     

Topology induced anomalous plasmon modes in metallic Möbius nanorings

We report on the theoretical investigation of plasmonic resonances in metallic Möbius nanorings. Half‐integer numbers of resonant modes are observed due to the presence of an extra phase π provided by the topology of the Möbius nanostrip. Anomalous plasmon modes located at the non‐orientable surface of the Möbius nanoring break the symmetry that exist in conventional ring cavities, thus enable far‐field excitation and emission as bright modes. The far‐field resonant wavelength as well as the feature of half‐integer mode numbers is constant to the change of charge distribution on the Möbius nanoring due to the topology of Möbius ring. Owing to the ultra‐small mode volume induced by the remaining dark feature, an extremely high sensitivity as well as a remarkable figure of merit is obtained in our numerical calculations for sensing performance. The topological metallic nanostructure provides a novel platform for the investigation of localized surface plasmon modes exhibiting unique phenomena for potential plasmonic applications.