Effect of size and morphology of Au nanostructures on boosting performance of organic photovoltaic devices: Plasmonic and non-plasmonic effects

We fabricated organic photovoltaic (OPV) devices containing various Au nanostructures mixed with hole-collecting buffer layer. The presence of the Au nanostructures results in enhancement of the external quantum efficiencies (EQE) at dissimilar wavelengths of visible light, which can be attributed to the modulated plasmonic absorption frequency of the Au nanostructures. In addition to this plasmonic effect induced by visible light absorption, an increase in the EQE was also found upon UV excitation, which can be attributed to scattering effects induced by Au particles. The optical response pattern of organic photovoltaic devices can be modulated in a wide range of visible and UV wavelengths, by controlling sizes and shapes of the Au nanostructures.     

First-principles study of plasmons in doped graphene nanostructures

The operating frequencies of surface plasmons in pristine graphene lie in the terahertz and infrared spectral range,which limits their utilization. Here, the high-frequency plasmons in doped graphene nanostructures are studied by the timedependent density functional theory. The doping atoms include boron, nitrogen, aluminum, silicon, phosphorus, and sulfur atoms. The influences of the position and concentration of nitrogen dopants on the collective stimulation are investigated,and the effects of different types of doping atoms on the plasmonic stimulation are discussed. For different positions of nitrogen dopants, it is found that a higher degree of symmetry destruction is correlated with weaker optical absorption. In contrast, a higher concentration of nitrogen dopants is not correlated with a stronger absorption. Regarding different doping atoms, atoms similar to carbon atom in size, such as boron atom and nitrogen atom, result in less spectral attenuation. In systems with other doping atoms, the absorption is significantly weakened compared with the absorption of the pristine graphene nanostructure. Plasmon energy resonance dots of doped graphene lie in the visible and ultraviolet spectral range.The doped graphene nanostructure presents a promising material for nanoscaled plasmonic devices with effective absorption in the visible and ultraviolet range.     

Extreme Ultraviolet Sources Generation by Using the Two-Color Multi-Cycle Weak Inhomogeneous Field

An efficient method for attosecond extreme ultraviolet source generation under the two-color multi-cycle weak pulse has been theoretically presented by using the concept of the plasmonic field enhancement in the vicinity of metallic nanostructures. The results show that by properly choosing the inhomogeneity of the two-color multi-cycle(20 fs) weak pulse(1013W/cm2), not only the harmonic cutoff has been extended, resulting in a broadband XUV continuum, but also the single short quantum path has been selected to contribute to the harmonic. As a result, two isolated XUV pulses with durations of 68 as and 66 as can be obtained.     

Inhomogeneous Double Optical Gating of High-Intensity Isolated Attosecond Pulse Generation in Crossed Metal Nanostructures

We propose and investigate an effective method for obtaining high-energy and high-intensity isolated attosecond pulses (IAPs) using the inhomogeneous double optical gating (DOG) technology in specifically designed metal nanostructures. First, using the homogeneous mid-infrared DOG technology modulated by a linearly near-infrared field, we obtain a harmonic yield of 2.5 orders of magnitudes higher than that from the single polarization gating (PG) technology. Further, introducing the crossed metal nanostructures along the driven and gating components, we can extend not only the harmonic cutoff but also enhance the harmonic yield attributed to the plasmonic field enhancement near the vicinity of metal nanostructures. As a result, we find a single harmonic plateau with smaller modulations. The supercontinuum is not very sensitive to the pulse duration of the near-infrared field, and the harmonic yields can be further enhanced with increase in the pulse intensity of the near-infrared field, showing a 108 eV supercontinuum with an intensity enhancement of 4 orders of magnitudes. Finally, by superposing the selected harmonics from the inhomogeneous DOG scheme, we obtain a 33 as SAP with an intensity increase of 4 orders of magnitudes.     

花状纳米金结构阵列的工艺制备与拉曼增强研究

基于纳米球光刻技术制备了一种花状纳米金结构阵列,经过PS509 nm球旋凃和ICP氧刻蚀,再通过镀金膜与高温退火工艺,纳米球阵列的表面被粗糙化,进而形成了一种鳞状的花状阵列 。FDTD仿真结果表明,制备的这种阵列具备很高的电磁场增强特性,主要的增强集中于纳间隙的边缘处。以罗丹明 6G染料为探针分子测试基底的拉曼效应,与金基底的拉曼信号相比,该纳米结构阵列拉曼增强效应明显,对罗丹明 6G的检测极限达到了10-6 mol/L的水平。     

不同Ag壳厚度Au@Ag纳米粒子的调控制备表征及表面增强拉曼光谱的效应

采用化学还原法制备了以Au为核、包覆Ag的双金属核壳Au@Ag纳米粒子,并成功地用于表面增强拉曼光谱(SERS)分析测试。通过改变制备液中Ag/Au的量比来调控Ag壳包覆厚度。采用透射电子显微镜(TEM)和紫外-可见光谱仪(UV-Vis)对Au@Ag纳米粒子的构貌进行表征。TEM显示明显存在核壳结构,且Ag壳层随Ag/Au的量比的增加而逐渐变厚;UV-Vis表明随着Ag/Au的量比的增加,Au@Ag纳米粒子出现了Au核与Ag壳吸收峰的2个等离子体共振峰,同时伴随着Au峰的蓝移和Ag峰的红移。以双甲脒为分析物,考察了不同Ag/Au的量比时的Au@Ag纳米粒子的SERS活性。结果表明,SERS活性随Ag/Au的量比的增加先增大后减小,在6∶5时其SERS增强效应最佳,此时Ag壳厚度约为6 nm。以对巯基苯胺(4-ATP)、结晶紫(CV)和双甲脒为分析测试对象,对比了Au@Ag、Ag、Au 3种基底的SERS活性。结果表明,所制备的Au@Ag纳米粒子的SERS活性要明显优于单纯的Au、Ag纳米粒子。     

Spatial polarization sensitivity of single Au bowtie nanostructures

Metallic bowtie nanostructures as plasmonic nanoantennas can create highly enhanced local fields when resonating with the incident light. With Au bowtie nanostructures fabricated by lithography method, we experimentally observed that the photoluminescence (PL) spatial profile from a single Au bowtie nanoantenna was strongly dependent on the excitation light polarization. While varying the incident light polarization, the spatial distribution of the PL intensity in the nanogap of an Au bowtie changed as predicted by the simulation results on the electromagnetic field enhancement distribution. The polarization feature of the PL intensity relative to the polarization direction of incident excitation light was also discussed. The study may find application in the design of polarization sensitive plasmonic sensors.     

Prospects of Utilizing Quantum Emitters to Control the Absorption of Non-Noble Plasmonic Metal Nanoparticles

Prospects of controlling the absorption of the cost-effective plasmonic metal nanoparticles (MNPs) Cu and Al using quantum emitters (QEs) are demonstrated semi-analytically. The resulting spectra are compared with the absorption of commonly used noble plasmonic metal nanoparticles Au and Ag under similar conditions. It is observed that Cu and Au based plasmonic nanoparticles exhibit largely similar exciton–plasmon Fano interaction signatures in addition to their similar spectral regions of operation (lower end of the visible range). Furthermore, the QE-enhanced maximum absorption (Fano maximum) of Cu based nanohybrids are seen to approach the maximum absorption level of isolated Au MNPs, with decreasing QE-Cu separation, increasing QE dipole element magnitude, and increasing medium permittivity, in the parameter region considered. This renders Cu based exciton–plasmon nanohybrids as more economical alternatives for Au MNPs and Au-based nanohybrids in absorption-based applications (such as thermoplasmonic), when stabilized in protective embedding media such as poly (methyl methacrylate) (PMMA).     

Optical bistability and multistability in a four-level quantum system in the presence of plasmonic nanostructure

In this paper, the effect of plasmonic nanostructure on behavior of optical bistability and multistability in a four-level quantum system embedded in a unidirectional ring cavity has been studied. It is found that the distance between plasmonic nanostructures and a four-level quantum system is varied from 4.4 nm to 14.4 nm and has an essential role for controlling the threshold of optical bistability and multistability. Moreover, obtained results show that the group velocity of pulse propagation through the medium is strongly depended on the distance between the plasmonic nanostructure and the four-level quantum system.     

Secondary plasmon resonance in graphene nanostructures

The plasmon characteristics of two graphene nanostructures are studied using time-dependent density functional theory (TDDFT). The absorption spectrum has two main bands, which result from π and σ + π plasmon resonances. At low energies, the Fourier transform of the induced charge density maps exhibits anomalous behavior, with a π phase change in the charge density maps in the plane of the graphene and those in the plane 0.3 ? from the graphene. The charge density fluctuations close to the plane of the graphene are much smaller than those above and beneath the graphene plane. However, this phenomenon disappears at higher energies. By analyzing the electronic properties, we may conclude that the restoring force for the plasmon in the plane of the graphene does not result from fixed positive ions, but rather the Coulomb interactions with the plasmonic oscillations away from the plane of the graphene, which extend in the surface-normal direction. The collective oscillation in the graphene plane results in a forced vibration. Accordingly, the low-energy plasmon in the graphene can be split into two components: a normal component, which corresponds to direct feedback of the external perturbation, and a secondary component, which corresponds to feedback of the Coulombic interaction with the normal component.     

Generation of isolated attosecond pulses in bowtie-shaped nanostructure with three-color spatially inhomogeneous fields

We theoretically investigate high-order harmonic generation in a two-color multi-cycle inhomogeneous field combined with a 27 th harmonic pulse. By considering a bowtie-shaped gold nanostructure, the spatiotemporal profiles of enhanced plasmonic fields are obtained by solving the Maxwell equation using finite-domain time-difference method. Based on quantum-mechanical and classical models, the effect of 27 th harmonic pulse, temporal profile of enhanced plasmonic field and inhomogeneity on supercontinuum generation are analyzed and discussed. As a result, broadband supercontinuum can be generated from our approach with optimized gap size of nanostructure. Moreover, these results are not sensitively dependent on the relative phase in the two-color field.     

Two‐Dimensionally Ordered Plasmonic and Magnetic Nanostructures on Transferable Electron‐Transparent Substrates

Discovery of new plasmonic behaviors from nanostructured materials can be greatly accelerated by the ability to prepare and characterize their near‐field behaviors with high resolution in a rapid manner. Here, an efficient and cost‐effective way is reported to make 2D periodic nanostructures on electron‐transparent substrates for rapid characterization by transmission electron microscopy. By combining nanosphere lithography with a substrate float‐off technique, large areas of electron‐transparent periodic nanostructures can be achieved. For this study, the synthesis of plasmonic nanostructures of Ag, magnetic nanostructures of Co, and bimetallic nanostructures of Ag–Co are investigated. Characterization of the materials by a combination of transmission electron microscopy, far‐field optical spectroscopy, and magnetization measurements reveals that this new approach can yield useful nanostructures on transparent, flexible, and transferable substrates with desirable plasmonic and/or magnetic properties.     

Nanocomposite ZnO/Au formation by pulsed laser irradiation

The ZnO/Au nanocomposite formation involves synthesis of Au and ZnO colloidal solutions by 532 nm pulse laser ablation of metal targets in deionized water followed by laser irradiation of the mixed colloidal solution. The transmission electron microscope (TEM) and high-resolution transmission electron microscope (HRTEM) images show evolution of spherical particles into ZnO/Au nanonetworks with irradiation time. The formation mechanism of the nanonetwork can be explained on the basis of near resonance absorption of 532 nm irradiation by gold nanoparticles which can cause selective melting and fusion of gold nanoparticles to form network. The ZnO/Au nanocomposites show blue shift in the ZnO exciton absorption and red shift in the Au plasmon resonance absorption due to interfacial charge transfer.     

Tunable multi-band terahertz absorber based on graphene nano-ribbon metamaterial

The tunable multi-band selective absorption effect with graphene nano-ribbon metamaterial is investigated. It is achieved by depositing a set of graphene nano-ribbons on a dielectric spacer backed with a metallic mirror. A dual-band and tri-band absorbers are designed to illustrate such multi-band selective absorption behavior. The designed graphene absorbers exhibit near-unity absorption at multiple resonance frequencies, which is attributed to the plasmonic resonance of graphene nano-ribbons with different widths. Moreover, the multiple resonance wavelengths can be tuned in a wide frequency range by changing the Fermi energy and the absorbers possess large angle insensitivity. Last, a Fabry-Perot model is employed to give a physical understanding of such multi-band selective absorption effect. It is believed that the conclusions may be useful for designing of next-generation graphene-based optoelectronic devices.     

Optical spectroscopy of graphene: From the far infrared to the ultraviolet

The unique electronic structure of graphene leads to several distinctive optical properties. In this brief review, we outline the current understanding of two general aspects of optical response of graphene: optical absorption and light emission. We show that optical absorption in graphene is dominated by intraband transitions at low photon energies (in the far-infrared spectral range) and by interband transitions at higher energies (from mid-infrared to ultraviolet). We discuss how the intraband and interband transitions in graphene can be modified through electrostatic gating. We describe plasmonic resonances arising from the free-carrier (intraband) response and excitonic effects that are manifested in the interband absorption. Light emission, the reverse process of absorption, is weak in graphene due to the absence of a band gap. We show that photoluminescence from hot electrons can, however, become observable either through femtosecond laser excitation or strong electrostatic gating.     

金银复合体系表面增强拉曼光谱分离

采用传统自组装技术在硅片表面进行金银纳米粒子的复合组装.以吡啶为探针分子,利用金银在不同激发光线下增强效应的不同,研究了不同波长的激发光下纯金、银以及复合组装时体系的SERS效应.结果表明在金银同时组装时的增强效应强于金弱于银,同时还通过一系列校正以及差谱方法分离出金银共存时SERS中金的增强效应,并进行了相关分析,结果表明在金银同时组装的复合体系中,金银之间产生一定的耦合作用.     

Strained graphene as a local probe for plasmon‐enhanced Raman scattering by gold nanostructures

We investigate with Raman spectroscopy how gold nanostructures of different shape, size and geometry locally modify a graphene cover layer through strain. The resulting phonon softening translates into frequency downshifts of up to 85 cm^–1 for the 2D‐mode of graphene. With spatially resolved and excitation dependent Raman measurements we demonstrate that the downshifted Raman peaks exclusively arise from strained graphene subject to plasmonic enhancement by the nanostructures. The signals arise from an area well below the size of the laser spot. They serve as a local probe for the interaction between graphene and intense light fields. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

基于石墨烯加载的不对称纳米天线对的表面等离激元单向耦合器

本文设计并数值研究了一种石墨烯加载的不对称金属纳米天线对结构.利用石墨烯费米能级的动态调控特性,实现了电控表面等离激元的单向传输.类似于传统的三明治型纳米天线结构,设计的不对称金属纳米天线对结构可以等效为两个共振的磁偶极子,由于磁偶极子辐射电磁波的干涉,将导致单向传输效应.通过计算腔中的电场分布,发现石墨烯的调谐能力与石墨烯区域的电场强度成正比关系.以上现象都可以通过等效电路模型进行理论解释.此外,该结构具有小尺寸、高效率、宽带宽和易于光电集成等优点,在未来的光子集成与光电子学领域将具有重要的应用.     

Plasmonic hot electron tunneling photodetection in vertical Au–graphene hybrid nanostructures

Plasmon‐induced hot‐electron generation provides an efficient way to convert light into electric current. The investigation of the optoelectronic response in two‐dimensional materials and metallic hybrid nanostructure attracts increasing research interest. Here, we present a tunneling effect of plasmonic hot electrons that is generated from Au nanoparticles, which can vertically tunnel through graphene monolayers. A strong photocurrent induced by the hot electrons was measured in this graphene‐based vertical photodetector with its intensity maximum reached at the plasmon resonance wavelength. The tunneling effect of plasmonic hot electrons was investigated by gradually increasing the incident laser power and bias voltage between the top and bottom electrodes. The dynamic attenuation of plasmonic hot electrons in an excited state was further investigated with multilayered graphene sheets. These results show that our vertical hybrid structure can function as an effective design for the tunneling photodetector, and enable the realization of complex nanophotonic devices that are based on graphene and other 2D materials, such as optical transistors and plasmonic hot‐electron sensors.

     

Fabrication and surface-enhanced Raman scattering (SERS) of Ag/Au bimetallic films on Si substrates

Ag films on Si substrates were fabricated by immersion plating and served as sacrificial materials for preparation of Ag/Au bimetallic films by galvanic replacement reaction. The formation procedure of films on the surface of Si was studied by scanning electron microscopy (SEM), which revealed Ag films with island and dendritic morphologies experienced novel structural evolution process during galvanic replacement reaction, and nanostructures with holes were produced within the resultant Ag/Au bimetallic films. SERS activity both of sacrificial Ag films and resultant Ag/Au bimetallic films was investigated by using crystal violet as an analyte. It has been shown that SERS signals increased with the process of galvanic substitution and reached intensity significantly stronger than that obtained from pure Ag films.