散射光谱的目标材质及比例反演研究

研究了基于散射光谱的点目标在远距离条件下表面材质及比例反演方法,旨在为空间碎片探测及预报提供数据参考。首先根据散射光谱的远距离目标探测物理模型,建立了基于散射光谱的目标参数反演物理模型,给出了基于最小二范数理论方法的目标表面材质及比例信息的反演算法,结合光源照射特性、目标材料表面光学反射特性、入射、反射及探测角等信息,利用双向反射分布函数(BRDF)的多级融合模型,表征复杂材料表面的光学反射特性,将BRDF中对应的面积量作为待反演参数,给出了目标表面材质及比例信息的反演算法;其次进行了实验验证,搭建了室内散射光谱探测及采集系统,进行了单一材质及多种材质不同比例的目标散射光谱探测及数据采集,经过对散射光谱数据进行预处理,截取有效波长范围为400～800 nm;结合理论分析及反演算法,对于四种材质组合的样品,进行了相同和不同比例组合的材质及比例反演,等比例反演结果最小误差为0.8%。最大误差为13.6%,平均误差为4.9%;不等比例反演结果最小误差为6%,最大误为12%,平均误差为9.25%;综合以上测试结果可以得出,反演平均误差最大为9.25%,考虑到入射光源稳定性有2.89%的误差,反...     

金纳米棒二聚体结构的Fano共振

等离激元金属纳米结构中的Fano共振，由于其在超灵敏传感、超材料、光开关和非线性光学器件等方面的潜在应用而引起了广泛的关注。但在单颗粒尺度下单个金属纳米二聚体结构的Fano共振的实验研究仍然很少。本研究基于单颗粒光谱技术从实验上探讨了二聚体结构产生的Fano共振现象。利用种子生长法制备了等离激元共振峰分别在1 060 nm和700 nm的一长一短金纳米棒，通过L-半胱氨酸分子的静电吸附自组装构建首尾相连的金纳米棒二聚体结构，在暗场显微系统中表征了金纳米棒二聚体耦合前后的散射光谱。结果表明，短金纳米棒的明偶极模式与长金纳米棒的暗四极模式间的相消干涉在660 nm处产生了明显的Fano共振谷，同时基于有限差分时域（FDTD）方法的理论模拟散射光谱与实验结果能够较好地符合。这种自组装金纳米棒二聚体在等离激元传感和探测等方面具有广阔的应用前景。     

D-核糖NIR-SERS光谱及其在金纳米棒表面吸附行为分析

本文采用种子生长法、利用双表面修饰剂制备了金纳米棒,其长径比为3.5:1。该金纳米棒的消光光谱显示:利用该方法制备的金纳米棒有两个表面等离子共振(SPR)峰,分别位于540nm和780nm处。其中780nm处的表面等离子共振峰靠近红外光谱区,可以与文中采用的激发光源(785nm激光)较好的匹配,从而有助于实现共振拉曼散射增强效应。本文以D-核糖(D-Ribose)为探测分子,基于金纳米棒进行了近红外表面拉曼散射(NIR-SERS)活性检测,从而获得了光谱重复性良好的NIR-SERS光谱图。同时,采用密度泛函理论(DFT),以B3LYP/6-31G和6-31G/LanL2DZ为基组函数,分别对D-核糖分子以及D-核糖分子与金原子形成的团簇进行结构优化和普通拉曼光谱(NR)计算,发现理论值和实验值符合较好。此外,文中对D-核糖的NIR-SERS谱带进行了分析和归属,发现当D-核糖分子吸附到金纳米粒棒上时,主要是以羟基上的氧原子(O9)吸附在金原子上而形成金属键。     

生物组织单光程光谱技术的理论研究

高灵敏度光谱检测技术在临床诊疗和组织光学参数测量中具有极其重要的意义。文章提出了一种差分调制激光光谱技术,将经过生物组织后的散射光与参考光的光程差转换为光谱信号的频率特征,通过相敏检测技术将不同频率的信号进行分离,从而实现生物组织散射光的光程分离。文章分析了差分调制激光光谱的机理及信号的谱特征,并基于文献中的生物组织散射光的光程分布,从理论上讨论了差拍信号的谱特征,即光源调制速率一定时,光谱信号中的主频成分位置只与散射光和参考光的光程差有关;生物组织对光信号的衰减系数会影响光谱信号中频率成分的能量强度分布。分析结果表明,差分调制激光光谱能对生物组织的光谱信号进行光程分离,从而实现生物组织的单光程光谱检测。     

连续激光辐照对三结砷化镓电池散射光谱的特性影响

太阳能电池作为一种高效的光电转化器,被广泛地应用于光伏发电系统中。激光作为一种高亮度光源辐照电池时,会导致其出现损伤,可利用电池的表面散射光谱特性,对其损伤程度进行判别。通过目标表面散射光谱测量系统,对激光辐照后的三结砷化镓电池散射光谱进行测量,并计算双向反射分布函数(BRDF)。其中测量系统主要由FX 2000和NIR 17型光纤光谱仪组成,针对电池表面的强镜反射特性,在实验中采用了入射角和反射角为30°的测量几何模型。原始三结砷化镓太阳能电池的结构主要包括减反射膜DAR层、顶电池GaInP层、中电池GaAs层和底电池Ge层,其散射光谱特征包括可见光谱段(500～900 nm)的吸收特性及近红外谱段(900～1 200 nm)的类周期振荡特性,在对连续激光辐照损伤后电池的光谱特性进行实验测量后,得到了损伤电池光谱BRDF的变化,并结合基于薄膜干涉理论的电池散射光谱模型,对各膜层损伤后的特征进行了分析。结果表明：DAR层的主要作用是降低光谱反射能量,对光谱曲线的特性影响较小;Ge层对光谱曲线形状基本无影响;电池散射光谱吸收和干涉等特征主要由GaInP层和GaAs层所引起,其中,GaIn...     

径向偏振光激发氧化石墨烯/金纳米棒复合基底的表面增强拉曼散射性能

探究径向偏振矢量光与氧化石墨烯/金纳米棒复合结构的相互作用,以提高表面增强拉曼散射性能。基于FDTD Solutions软件,得到氧化石墨烯/单金纳米棒复合基底在径向偏振光激发下的表面增强拉曼散射增强因子达到10~8,比相同条件下线偏振光激发的大6个数量级。这种性能提高的物理机制源于径向偏振光激发金纳米棒的电磁增强与氧化石墨烯产生的本征化学增强。进一步详细讨论了径向偏振光激发下氧化石墨烯厚度、金纳米棒数量和排列方式对表面增强拉曼散射性能的影响。基于径向矢量光场激发多功能基底的表面增强拉曼散射性能调控在生物化学、食品安全与传感检测等领域具有巨大的应用潜力。     

电子能量损失谱探测银纳米棒与介质层强耦合的数值模拟

表面等离激元与量子发射体间的强耦合现象通常通过散射、吸收以及荧光等远场光谱探测方法进行研究.利用高度聚焦的电子束,电子能量损失谱能够实现亚纳米尺度的局域探测,可以更加有效地研究强耦合现象.本文在理论上分别模拟了银纳米棒、介质材料以及介质层包裹银纳米棒复合结构的电子能量损失谱.得到了可以与实验结果比拟的银纳米棒表面等离激元的电子能量损失谱.在上述复合结构的电子能量损失谱中观察到了谱峰的拉比劈裂,探究了银纳米棒尺寸对拉比劈裂的影响.分别在红外、可见光波段讨论了介质层的元激发与银纳米棒偶极辐射及高阶非辐射表面等离激元模式间的强耦合现象,从损失谱的空间分布成像角度探讨了强耦合引起的杂化等离激子(plexciton)的形成.本研究对强耦合现象的进一步实验和理论研究具有指导意义.     

基于金纳米粒子的光谱分析法进行单细胞探测

在过去的几十年中,等离子纳米粒子,尤其是金纳米粒子(AuNPs),由于其独特的局部表面等离子体共振(LSPR)特性,金纳米颗粒非常适合高度传导定域在表面的化学或物理刺激产生的光信号,已被广泛应用于生物检测与成像。包括单细胞光谱分析与成像。基于光吸收和弹性光学方法散射,阐述了利用光谱方法进行的单细胞光学探测的进展应用和纳米系统表现出新的特性。论述了基于AuNPs的细胞内环境光谱分析与探测,对在单细胞水平上进行的细胞动态实时测量的基本原则和与光互动独特的相关方法进行了描述。重点放在单细胞光谱检测的原则、方法及这些方法的优点和挑战,并阐述了最近在这一领域的研究进展,内容包括细胞和亚细胞环境的探测、细胞应答诱导细胞凋亡过程探测、生物分子识别和量化、药物传递及释放、癌症诊断及治疗等。给出了未来的挑战和努力方向。     

外围介质介电常数对金纳米棒光学性质影响的数值模拟

采用电化学方法制备出悬浮胶体金纳米棒。在室温下测得其紫外-可见吸收光谱和荧光发射光谱。结合准静电场理论与散射理论对金纳米棒的光学特性进行了数值模拟。计算结果表明,由于金纳米棒形状的各向异性,吸收截面与散射截面均出现两个共振峰,分别对应于横截方向与长轴方向的表面等离子共振。对于几何形状一定的金纳米棒,在外围介质介电常数从1.5增加到2.5的过程中,两个共振吸收峰均增强并非线性红移。然而对于散射光谱,短波方向的共振峰线性红移,强度变化微弱;长波方向的共振峰减弱并非线性红移。     

金纳米棒复合体的消光特性

金属纳米颗粒局域表面等离激元共振时能够产生消光和近场增强效应已经成为国内外研究的热点. 应用时域有限差分法对L形纳米棒与普通纳米棒构成的金纳米棒复合体的消光光谱及其近场增强和电流矢量密度分布进行了研究. 计算结果表明, 普通纳米棒和L形纳米棒二聚体的光谱响应与纳米棒间的间距有关, 而金纳米棒复合体的消光光谱可通过调整L形纳米棒与普通纳米棒间的间距、L形纳米棒的臂长度以及普通纳米棒的长度进行调谐. 此外金纳米棒复合体可以分解成L形纳米棒二聚体和普通纳米棒二聚体两个部分, 通过分别改变L形纳米棒的臂长和普通纳米棒的长度, 对比L形纳米棒二聚体和普通纳米棒二聚体间的共振峰位置变化, 可以更直观地了解金纳米棒复合体消光光谱线型的变化. 这些结果可用于指导金纳米棒复合体纳米光子器件的设计, 以满足其在表面增强拉曼散射和生物传感等方面应用.     

The Aggregation Enhanced Photoluminescence of Gold Nanorods in Aqueous Solutions

The photoluminescence (PL) properties of single gold nanorod (AuNR) under one-photon excitation (OPE) have been reported recently. In this work, the PL of AuNRs in aqueous solutions were studied with OPE of 514 or 633 nm to characterize the emissions of transverse and longitudinal surface Plasmon resonance (TSPR and LSPR) bands, because the AuNRs aqueous solution was frequently used in bio-medical applications. We found that under 514 nm OPE the TSPR emissions of four groups of AuNRs with different aspect ratios in aqueous solutions were all strong dominating the PL emission with the quantum yield (QY) of 10^?4, which is at least three orders of magnitude higher than that of single AuNR. We further found that the aggregate was the basic form of AuNRs in aqueous solution and living cells, measured by the elastic light scattering and transmission electron microscopy measurements. The Plasmon coupling particularly the TSPR coupling between the neighbored AuNRs in aggregates enhanced the PL and increased the QY, because the conjugation of the rod side to side was a main aggregate mode. Under 633 nm OPE, only LSPR emissions of AuNRs aqueous solutions occurred with the QY level of 10^?5 which is very similar to that of singe AuNR, because of the negligible LSPR coupling.     

Near-field and far-field modeling of scattered surface waves. Application to the apertureless scanning near-field optical microscopy

The detection of surface waves through scanning near-field optical microscopy (SNOM) is a promising technique for thermal measurements at very small scales. Recent studies have shown that electromagnetic waves, in the vicinity of a scattering structure such as an atomic force microscopy (AFM) tip, can be scattered from near to far-field and thus detected. In the present work, a model based on the finite difference time domain (FDTD) method and the near-field to far-field (NFTFF) transformation for electromagnetic waves propagation is presented. This model has been validated by studying the electromagnetic field of a dipole in vacuum and close to a dielectric substrate. Then simulations for a tetrahedral tip close to an interface are presented and discussed.     

Shape Matters: A Gold Nanoparticle Enabled Shape Memory Polymer Triggered by Laser Irradiation

With incorporation of gold nanoparticles, i.e., nanorods (AuNR) and nanospheres (AuNS), into a polyurethane‐based shape‐memory polymer (SMP) EG‐72D matrix, SMP nanocomposite films capable of being remotely triggered by low‐power laser are fabricated and characterized using UV‐vis‐NIR spectroscopy, X‐ray scattering, and dynamic mechanical analysis (DMA). It is demonstrated that, with incorporation of very low concentration of gold nanorods (≈0.1 wt%), the mechanically programmed EG‐72D/AuNR nanocomposite presents rapid response to low power laser irradiation (785 nm, ≈10 mW). Comparative studies on the laser irradiation response of EG‐72D/AuNS and EG‐72D/AuNR nanocomposite films suggest that AuNRs have significantly higher photothermal conversion efficiency than AuNS and on‐resonance laser irradiation, matching the wavelength of the incident laser with the longitudinal plasmon resonance of AuNR, is necessary to induce the fast response of gold nanoparticle enabled SMP nanocomposites.     

The dynamic angle-limited integrated scattering (DALIS) method for measuring scattering of light from optical surfaces with random roughness

A new and simple dynamic angle limited integrated scattering (DALIS) method is developed to examine optically smooth reflective surfaces with defined surface form. Our experimental results from two systems show advantages over conventional angle resolved scattering measurement (ARS) methods. By collecting scattered light in a given solid angle, our methods do not require a detection unit with an extremely large dynamic range. Unlike in the common ARS measurement method, here we use a simple linear translation stage to scan scattered light. The power spectrum density function and the autocorrelation function of the surface roughness can be recovered from the measured scattering pattern. This method can be applied to in-workshop inspection of optical polishing processes.     

Wave scattering functions and their application to multiple scattering problems

Scattering functions arise naturally in standard treatments of the effects of a material object or surface embedded in a uniform field. The most commonly used scattering function describes the far-field modulation imparted at large distances to a spherical wavefront eminating from the scatterer. The purpose of this is to develop the properties of the spectrum of scattered plane waves as an exact generalized scattering function. The linearity of the wave equations guarantees that such a representation exists; moreover, it is possible to derive the generalized scattering function from the far-field scattering function by analytic continuation. Although these properties are known, recent theoretical developments have motivated us to reexplore the interrelations among the far-field scattering function, the Green's function and various forms of the generalized scattering function as well as the symmetry properties of the generalized scattering function imposed by reciprocity. For multiple-scattering objects that can be separated by parallel planes, a system of difference equations is developed that fully accommodates the mutual interaction among the scatterers. The mutual interaction equations were developed earlier, but we show here that they can be transformed into the form that would be obtained by using the Foldy-Lax-Twersky formalism. This reinforces the equivalence between wave-space and configuration space formulations of the scattering problems.     

Speckle diagnostics of multiple scattering media with the use of frequency-modulated laser radiation

A method for probing randomly inhomogeneous multiple scattering media with the use of frequency-modulated laser radiation is considered. The method is based on analysis of the dependence of the blinking index of time-averaged speckles formed upon scattering of the probing radiation in a medium on the frequency modulation depth of the probing radiation. In the case of a binary frequency modulation, the blinking index of the detected speckle-modulated radiation is determined by the cosine Fourier transform of the probability density of the optical path-length difference of partial components of the scattered field in the probed medium. The values of the probability density of the optical path-length difference reconstructed with the use of the proposed method from the measured blinking index of speckles for model scattering media (fluoroplastic layer and layer of TiO₂ particles on a glass substrate) are in a good agreement with the results of statistical simulation of the probing radiation transfer in multiple scattering media.     

Study of electrical field distribution of gold-capped nanoparticle for excitation of localized surface plasmon resonance

The specific optical characteristics which can be observed from noble metal nanostructured materials such as nanoparticles and nanoislands have wide variety of applications such as biosensors, solar cells, and optical circuit. Because, these noble metal nanostructures induce the increment of light absorption efficiency by the enhancing effect of electrical field from localized surface plasmon resonance (LSPR) excitation. However, the enhancing effects of electrical field from LSPR using simple structured noble metal nanostructures for several applications are not satisfactory. To realize the more effective light absorption efficiency by the enhancing effect of electrical field, quite different noble metal nanostructures have been desired for applying to several applications using LSPR. In this study, to obtain the more effective enhancing effect of electrical field, conditions for LSPR excitation using a gold-capped nanoparticle layer substrate are computationally analyzed using finite-difference time-domain (FDTD) method. From the previous research, LSPR excitation using such gold-capped nanoparticle layer substrates has a great potential for application to high-sensitive label-free monitoring of biomolecular interactions. For understanding of detailed LSPR excitation mechanism, LSPR excitation conditions were investigated by analyzing the electrical field distribution using simulation software and comparing the results obtained with experimental results. As a result of computational analysis, LSPR excitation was found to depend on the particle alignment, interparticle distance, and excitation wavelength. Furthermore, the LSPR optical characteristics obtained from the simulation analysis were consistent with experimentally approximated LSPR optical characteristics. Using this gold-capped nanoparticle layer substrate, LSPR can be excited easily more than conventional noble metal nanoparticle-based LSPR excitation without noble metal nanoparticle synthesis. Hence, this structure is detectable a small change of refractive index such as biomolecular interactions for biosensing applications.     

金银三层纳米管局域表面等离激元共振特性研究

相对于单一金属纳米材料,二金属复合纳米材料具有更大的潜在应用价值.基于时域有限差分方法,研究了SiO₂-Ag-Au和SiO₂-Au-Ag二金属三层纳米管的消光光谱,并对其局域表面等离激元共振(Localized Surface Plasmon Resonance,LSPR)特性进行了分析.研究发现,内核尺寸变大将导致上述两种金属纳米管LSPR峰红移;内层金属及外层金属壳层厚度增大均会导致其LSPR峰蓝移.银壳厚度变化对纳米管LSPR的调制作用大于金壳厚度变化造成的影响.上述现象可以利用等离激元杂化理论及自由电子和振荡电子变化的竞争机制进行分析.     

Determination of the Surface Facets of Gold Nanorods in Wet‐Coated Thin Films with Grazing‐Incidence Wide Angle X‐Ray Scattering

This work studies the surface facets of gold nanorods (AuNRs) in wet‐coated nanoparticle thin films with synchrotron‐light‐based grazing‐incidence wide angle X‐ray scattering (GIWAXS), which provides statistically relevant results on many nanoparticles. Air‐brush spraying deposits the monodisperse AuNRs into sparse monolayers where the long axis of rods is parallel to the substrate surface. It is found that the crystalline facets of individual AuNRs in the sparse monolayer are all in the same orientation, as indicated by narrow azimuthal widths of (200) reflections, over a macroscopic scale comparable to the substrate. This alignment is probably due to the rods' sitting on high‐index surface facets such as (520) and (250). A quantitative analysis of the angles between bulk facets and the surface facets leads to a “nested‐octagon” model for the cross sections of AuNRs: shell octagon with high‐index crystalline facets (520), (5‐20), (2‐50), (‐2‐50), (‐5‐20), (‐520), (‐250), and (250), and core octagon consisting of low‐index crystalline facets (100), (1‐10), (0‐10), (‐1‐10), (‐100), (‐110), (010), and (110).