基于多形貌银纳米颗粒的多波长相干随机激光研究

采用溶剂热法分别制备了球形银纳米颗粒和多形貌银纳米颗粒,其中球形银纳米颗粒具有400 nm的窄带等离激元共振峰,而多形貌银纳米颗粒的共振区间在400～700 nm之间,将它们分别掺入R6G与PVP的混合溶液中,利用旋涂法在玻璃基板上制备银纳米颗粒嵌入染料掺杂聚合物薄膜随机激光器。采用纳秒脉冲激光进行随机激光泵浦实验,实验结果表明球形银纳米颗粒染料掺杂聚合物薄膜只有自发辐射峰,而多形貌银纳米颗粒染料掺杂聚合物薄膜具有线宽<0.8 nm的相干随机激光发射光谱,其阈值为1.9 mJ·cm-2, 这可能是由于银纳米颗粒的等离激元共振区间与R6G的发射光谱重叠,支持局域等离激元效应的形成,明显的局域场增强有效地改善了与附近分子的相互作用,从而激发了更多的辐射光子,促进了高增益的形成。进一步,利用多形貌银纳米颗粒在银纳米颗粒染料掺杂聚合物薄膜中随机分布的特性,通过改变泵浦位置,实现了20 nm范围内的随机激光输出波长的调控,具体输出范围为590.1～610.4 nm。认为这是由于多形貌银纳米颗粒在不同位置的组成和分布不同,改变了表面等离激元的相互作用和光子的散射能力,从而形成不同的增益效应和不同的封闭光振荡路径。此外,考虑到多形貌银纳米颗粒的共振波长较宽,探究了其用于输出其他颜色光的可能性。以与上述银纳米颗粒R6G染料掺杂聚合物薄膜相似的制备方法,制备了多形貌银纳米颗粒掺杂DCJTB染料聚合物薄膜,并且进行随机激光泵浦实验。结果表明,可以有效的产生波长为675 nm,半高宽<0.8 nm的相干红光随机激光,并且阈值仅为0.98 mJ·cm-2。研究结果在宽带可调谐随机激光器研究以及多色随机激光器研究领域具有重要的参考价值。     

基于递归T矩阵的离散随机散射体散射特性研究

本文根据电磁场矢量球波函数多极点展开原理及矢量叠加定理提出了递归T矩阵算法的矢量形式,并且基于矢量递归T矩阵算法建立了多散射球模拟离散随机散射体散射的三维电磁散射模型.通过计算不同尺寸、随机分布散射球的散射以及分析散射球间的高阶散射效应,结果表明:矢量递归T矩阵算法具有很高的计算精度,算法中包含多散射体间的高阶散射效应,因此能够精确计算多散射体总的散射效应.本文所建模型可应用于土壤湿度探测工程中评估地表下掩埋离散随机散射体散射对雷达回波信号产生的影响.     

Gravitational scattering of electromagnetic radiation

The scattering of electromagnetic radiation by linearized gravitational fields is studied to second order in a perturbation expansion. The incoming electromagnetic radiation can be of arbitrary multipole structure, and the gravitational fields are also taken to be advanced fields of arbitrary multipole structure. All electromagnetic multipole radiation is found to be scattered by gravitational monopole and time-varying dipole fields. No case has been found, however, in which any electromagnetic multipole radiation is scattered by gravitational fields of quadrupole or higher-order multipole structure. This lack of scattering is established for infinite classes of special cases, and is conjectured to hold in general. The results of the scattering analysis are applied to the case of electromagnetic radiation scattered by a moving mass. It is shown how the mass and velocity may be determined by a knowledge of the incident and scattered radiation.This work was supported in part by the National Aeronautics and Space Administration and the National Science Foundation. It incorporates some of the results of the first author's doctoral dissertation at the University of Pittsburgh.     

Substrate-Modulated Electromagnetic Resonances in Colloidal Cu2O Nanospheres

Dielectric nanoparticles are expected to complement or even replace plasmonic nanoparticles in many optical and optoelectronic applications, because they exhibit small absorption losses and support strong electric and magnetic resonances simultaneously. Dielectric nanoparticles need to be deposited on various substrates in many applications. Understanding the substrate effect on the electromagnetic resonances of dielectric nanoparticles is of great importance for engineering their resonance properties and designing optical devices. In this study, moderate-refractive-index cuprous oxide nanospheres with uniform sizes and shapes are synthesized. The scattering spectra and images of the nanospheres deposited on three types of substrates are analyzed experimentally and theoretically. When supported on indium tin oxide–coated glass slides and Si wafers, the color of the nanospheres varies from blue, cyan, green, yellow, orange and red, covering almost the entire visible region. When deposited on gold films, the electromagnetic resonances of the nanospheres redshift intensively and a new effective magnetic resonance mode appears. The enhanced Raman scattering reveals that large electromagnetic field enhancements are produced in the gap region between the nanosphere and the substrate. The results shed light on the manipulation of the electromagnetic responses of dielectric nanoparticles and the design of dielectric metamaterials in the presence of various substrates.     

Boundary integral equation method for analysis of light scattering by 2D nanoparticles

The scattering of a plane electromagnetic wave by 2D nanoparticles is simulated using the boundary integral equation method. The accuracy and smoothness of the solution are improved by applying Hermitean interpolants for discretization. The accuracy of the numerical approach used in this paper is comparable to the Mie classical solution for scattering by a circular cylinder. It is shown that laser radiation incident on silver nanoparticles generates plasma resonances, giving rise to peak values of the extinction cross section and considerably enhancing the local electromagnetic field on the surface.     

Effect of radiation on dust particles in orbital resonances

The effect of electromagnetic radiation on the dynamics of arbitrarily shaped cosmic dust particles is investigated. The paper concentrates on the motion of dust grains near commensurability resonances with a planet—mean-motion resonances—and possible capture of the grains in the resonances. A particle is in resonance with a planet when the ratio of the mean motions of the two objects is a ratio of two small integers.

The most fundamental properties of the orbital evolution of spherical dust particles in the mean-motion resonances are shortly rederived: the solar wind effect is also included and the existing result is improved. The results for spherical particles are compared with the detailed numerical calculations for nonspherical particles. It is shown that the fundamental results valid for spherical grains do not hold, in general, for nonspherical particles. While spherical particles are always characterized by the secular decrease of the semi-major axes near mean-motion resonances, this may not be true for nonspherical particles. Nonspherical grains may exhibit an increase of the semi-major axes before capturing in the mean-motion resonances. This is caused by the effect of electromagnetic radiation on nonspherical dust grains. The eccentricities of spherical particles in the exterior resonances approach a limiting value, but nonspherical grains may not follow this behaviour. The interior resonances are characterized by a systematic decrease of eccentricity for spheres, but various behaviours exist in the case of irregularly shaped particles.

The motion of a nonspherical dust particle under the action of electromagnetic radiation may be characterized by a small change of the semi-major axis during a long-time interval, but the particle is not captured in any mean-motion resonance. This kind of motion does not exist for spherical grains.     

Toroidal dipole‐induced transparency in core–shell nanoparticles

The scattering of nanoparticles plays a profound role in the recently flourishing fields of plasmonics and metamaterials. However, current investigations into nanoparticle scattering are based on the electric and magnetic resonances only, where their toroidal counterparts are usually not considered. The inclusion of toroidal terms can render new explanations for some fundamental scattering properties and thus may stimulate further breakthroughs in both scattering‐related basic researches and applications. Here we revisit the most fundamental problem of Mie scattering by individual spherical nanoparticles and show that compared to conventional interpretations in terms of electric and magnetic responses, the roles played by their toroidal counterparts are indispensable. Based on the demonstration of efficient toroidal dipole excitation in homogeneous dielectric particles, we reveal that the extensively studied scattering transparencies of core–shell nanoparticles can actually be classified into two categories: (i) the trivial transparency with no effective multipole excitations and (ii) the non‐trivial transparency induced by the destructive interferences of excited electric and toroidal multipoles. The incorporation of toroidal multipoles offers new insights into the study of nanoparticle scattering in both near and far fields, which may shed new light on many applications, such as biosensing, imaging, nanoantennas, photovoltaic devices, and so on.

     

Distorted wave theory of scattering of nucleons with intermediate energies on nuclei

In the context of nonrelativistic theory in the distorted wave approximation, a three-dimensional form of analytical expression for the differential cross section of scattering of nucleons with intermediate energies on atomic nuclei is derived. In the context of this theory, the main parameters of elastic scattering of protons with incident energy of 1 GeV on the ²⁰⁸Pb nucleus are determined. For inelastic scattering of protons with nuclear surface vibrations, giant multipole resonances in the excited nucleus are investigated for the collective nucleus model. The energy losses of the scattered proton are calculated together with the energies of giant dipole and quadrupole resonances and nuclear surface vibration energy. This allows the deformation parameter of the excited nucleus to be calculated.     

Size characteristics of surface plasmons and their manifestation in scattering properties of metal particles

The change of the scattering properties of sodium, gold and silver spherical particles with size is discussed in the context of surface multipolar plasmon resonances. The presented surface plasmon size characteristics are abstracted from the quantity which is observed and deliver multipolar plasmon resonance frequencies and plasmon damping rates in the form of a continuous function of particle radius. The performed analysis of the plasmon dispersion relation is analogous to the problem of surface plasmon localized at a semi-infinite, flat metal/dielectric interface.Correlation between the multipolar plasmon resonance parameters, and the spectroscopic optical properties of conductive nanoparticles appearing as peaks in the measurable light intensities is analyzed. We discuss the fact, that such peaks arise from interference of all the electromagnetic fields contributing to the measured intensity, and not solely to the fields due to surface plasmon multipolar modes.We describe the results of light scattering experiment in orthogonal polarization geometries with use of spontaneously growing sodium droplets. The polarization geometry of the experiment allows for distinct separation of resonant contribution of dipole and quadrupole plasmon TM mode contributions to the measured intensities as a function of size.Predictions concerning size characteristics for dipole and quadrupole plasmons are compared with the results of light scattering experiments using spherical sodium droplets (our results) and gold and silver particles in suspension [other authors: Sönnichsen C, Franzl T, Wilk T, von Plessen G, Feldmann J. Plasmon resonances in large noble-metal clusters. New J Phys 2002; 4:93.1–8; Haiss W, Thanh NTK, Aveyard J, Fernig DG. Determination of size and concentration of gold nanoparticles from UV–vis spectra. Anal Chem 2007; 79:4215–21; Njoki PN, Lim I-IS, Mott D, Park H-Y, Khan B, Mishra S, et al. Size correlation of optical and spectroscopic properties for gold nanoparticles. J Phys Chem C 2007; 111:14664–9; Mock JJ, Barbic M, Smith DR, Schultz DA, Schultz S. Shape effects in plasmon resonance of individual colloidal silver nanoparticles. J Chem Phys 2002; 116:6755–9].     

Interaction between plasmonic nanoparticles revisited with transformation optics

The interaction between plasmonic nanoparticles is investigated by means of transformation optics. The optical response of a dimer can be decomposed as a sum of modes whose resonances redshift when the nanoparticles approach each other. The extinction and scattering cross sections as well as the field enhancement induced by the dimer are derived analytically taking into account radiation damping. Interestingly, some invisibility dips occur in the scattering spectrum and originate from a destructive interference between each surface plasmon mode.     

Computer programs for light scattering by particles with inclusions

We present a comparison of computational results from light scattering by spherical particles with inclusions. The different simulation methods like the T-matrix method, multiple multipole method and the method of separation of variables are presented shortly. Exemplary numerical simulations involve scattering by particles with one or two spherical inclusions and scattering by particles with non-spherical inclusions.     

Quantized media with absorptive scatterers and modified atomic emission rates

Modifications in the spontaneous emission rate of an excited atom that are caused by extinction effects in a nearby dielectric medium are analyzed in a quantummechanical model, in which the medium consists of spherical scatterers with absorptive properties. Use of the dyadic Green function of the electromagnetic field near a dielectric sphere leads to an expression for the change in the emission rate as a series of multipole contributions for which analytical formulas are obtained. The results for the modified emission rate as a function of the distance between the excited atom and the dielectric medium show the influence of both absorption and scattering processes.     

A review of the effects of light scattering on the dynamics of irregularly shaped dust grains in the Solar System

The various aspects of the interaction of electromagnetic radiation with cosmic dust particles are discussed. In particular, attention is paid to discrepancies between optical and physical behavior of realistically shaped particles and volume equivalent homogeneous spheres. The dynamical evolution of morphologically non-identical particles which are driven by gravity, electromagnetic radiation and the Lorentz forces can dramatically differ. Although spherical particles often enable analytical calculations, an orbital evolution of spheres cannot be considered as a representative evolution for real cosmic dust particles. The effect of electromagnetic radiation on the motion of dust grains plays a crucial role here. While irregularly shaped interstellar dust particles may be captured in the Solar System, the spherical particles will not survive due to close encounters with the Sun. Spherical grains can be captured almost only in the evaporation region (in the vicinity of the Sun), where they are destroyed due to high temperatures. The spherical dust particles ejected from comets will monotonously inspiral toward the Sun subject to the Poynting-Robertson effect. However, the non-spherical particles of the same origin may be temporarily stabilized at some heliocentric distances and thus their lifetime may be much longer than that for the Mie spheres. Some dust particles may also be captured in mean-motion resonances with planets (commensurability resonances). While spherical particles are always characterized by the secular decrease of the semi-major axes near mean-motion resonances, this may not be true for non-spherical particles. Resonant captures of arbitrarily shaped dust grains exist for exterior and interior mean-motion resonances with planets.     

镍纳米球腔阵列上吸附分子拉曼散射的表面增强效应

通过聚苯乙烯纳米球为模板制备了规则排列的镍纳米球腔阵列。研究结果表明吸附于镍纳米球腔内的对巯基苯胺的拉曼散射可被极大增强。拉曼散射的表面增强被归因于纳米球腔阵列的协同表面等离子体共振与光的耦合导致的电磁场增强以及纳米球腔结构对电磁场的聚焦效应而使球腔内电磁场能量密度的增大。     

Evolution of terahertz conductivity in ZnSe nanocrystal investigated with optical-pump terahertz-probe spectroscopy

The unique optical properties of nanoparticles are highly sensitive in respect to particle shapes, sizes, and localization on a sample. This demands for a fully controlled fabrication process. The use of femtosecond laser pulses to generate and transfer nanoparticles from a bulk target towards a collector substrate is a promising approach. This process allows a controlled fabrication of spherical nanoparticles with a very smooth surface. Several process parameters can be varied to achieve the desired nanoparticle characteristics. In this paper, the influence of two of these parameters, i.e. the applied pulse energy and the laser beam shape, on the generation of Si nanoparticles from a bulk Si target are studied in detail. By changing the laser intensity distribution on the target surface one can influence the dynamics of molten material inducing its flow to the edges or to the center of the focal spot. Due to this dynamics of molten material, a single femtosecond laser pulse with a Gaussian beam shape generates multiple spherical nanoparticles from a bulk Si target. The statistical properties of this process, with respect to number of generated nanoparticles and laser pulse energy are investigated. We demonstrate for the first time that a ring-shaped intensity distribution on the target surface results in the generation of a single silicon nanoparticle with a controllable size. Furthermore, the generated silicon nanoparticles presented in this paper show strong electric and magnetic dipole resonances in the visible and near-infrared spectral range. Theoretical simulations as well as optical scattering measurements of single silicon nanoparticles are discussed and compared.     

Method for Describing the Angular Distribution of Optical Radiation Scattered by a Monolayer of Ordered Spherical Particles (Normal Illumination)

We have developed a method for describing the angular distribution of intensity of radiation scattered by a monolayer of homogeneous spatially ordered monodisperse spherical particles normally illuminated by a plane circularly polarized electromagnetic wave. The method is based on the quasicrystalline approximation (QCA) of the theory of multiple scattering of waves (TMSW) using the multipole expansion of fields and the tensor Green function in vectorial spherical wavefunctions. The method is applied for analyzing the characteristics of radiation scattered by a partially ordered monolayer and a monolayer with a nonideal lattice. The results of calculations are compared with the available experimental data on the position of the first-order diffraction peak on the angular and spectral dependences of the intensity of radiation scattered by a closely packed monolayer with a nonideal triangular lattice of SiO₂ particles. Good conformity of the results has been established.     

Observation of phase-matched electromagnetic scattering in an active dielectric cylinder

A theoretical investigation of oblique plane-wave electromagnetic scattering in an active dielectric cylinder predicted the existence of anomalous resonances at discrete plane-wave angles of incidence. These resonances may be understood as being due to a leaky-wave phase-matching boundary condition. Experiments were performed with active dielectric cylinders to confirm the existence of discrete resonances. Cross coupling between TE and TM modes was clearly detected for both active and passive scattering. Enhancement of active scattered field intensities was observed in experiments with finite-diameter pump and probe laser beams. Optical pumping of a dye solution was used to provide the gain.     

Electromagnetic transparency and slow light in an isotropic 3D optical metamaterial, due to Fano-like coupling of Mie resonances in excitonic nano-sphere inclusions

A three dimensional isotropic metamaterial is proposed and theoretically studied, which is composed of excitonic spherical nanoparticles in a dielectric host and exhibits electromagnetic transparency and slow light effects in optical regime. The approach is different from the conventional methods of realizing classical Electromagnetically Induced Transparency (EIT) or plasmon induced transparency effects, which are usually based on the interaction of dark and bright states of the medium plasmonic constituents. Instead, it is based on the Fano-like coupling of Mie resonances in the spherical inclusions, resulting from sharp and strong excitonic resonance of the particles. Using the Extended Maxwell Garnett effective medium approximation for calculating the effective electromagnetic parameters of the proposed metamaterial structure, it is shown that EIT-like effects can be produced, such as steep normal dispersion profiles within narrow transparency windows, resulting in high values of group index of refraction on the order of several thousands and figure of merit values around 10, near the excitonic resonance of the nanoparticle inclusions in UV region.     

Plasmon‐Enhanced Second‐ and Third‐Order Harmonic Generation in Spherical Free‐Electron Nanoclusters with Diffuse Surface

The nonlinear scattering of a laser pulse off spherical nanoclusters with free electrons and with a diffuse surface is examined in the collisionless hydrodynamics approximation in the framework of perturbation theory with respect to the laser pulse intensity, as well as of the steady‐state approximation. In a previous publication [S.V. Fomichev and W. Becker, Phys. Rev. A 81 , 063201 (2010)] we reported the full nonlinear hydrodynamic model of forced collective electron motion confined to a cluster with diffuse surface and introduced two different perturbation theories corresponding to different laser intensity regimes. In the current paper, in the framework of this hydrodynamic model we focus on the properties of plasmon resonance‐enhanced third‐harmonic generation in a spherical cluster and its dependence on the shape of its diffuse surface whose role increases for nonlinear processes. At the same time, the quadrupole second‐harmonic generation in a spherical cluster is also inspected as a necessary intermediate step. Both cold metal clusters in vacuum or in a dielectric surrounding and hot laser‐heated and laser‐ionized clusters are considered within the same approach for a wide range of the fundamental laser frequency. Nonlinear laser excitation of the dipole plasmon Mie resonance in spherical clusters, as well as of other respective multipole plasmon resonances is investigated analytically and numerically in detail (position, width, and strength) versus the cluster‐surface diffuseness, the outer ionization degree in charged clusters, the electron‐density diffuseness, and their interplay. Under certain conditions, depending on the various cluster parameters, different secondary nonlinear resonances are found. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Ku波段球体目标系的电磁复合散射研究

研究了球形目标之间的电磁相互作用,得到了目标二次散射场的表达式,给出了目标的复合散射场以及双站复合散射截面,并在Ku波段进行了数值仿真.结果表明：目标的尺寸对前向散射和后向散射均有较大的影响,周围目标的影响呈现出一定的周期性,二次散射随着目标间距的增大而减小,周围目标离前向散射方向越近,对前向散射的影响也越大.目标的二次散射场与一次散射场强度之比在10^-4数量级以上.在研究多粒子的相互影响时,周围的粒子可近似看作尺寸一定的粒子.利用所得结果以及坐标变换可以研究三维体系内粒子间的电磁相 关键词： 散射截面 二次电磁散射 电磁相互作用