Purely quadratic dispersion of surface plasmon in Ag/Ni(111): the influence of electron confinement

Surface plasmon dispersion in nanoscale thin Ag films deposited onto the Ni(111) surface was investigated by angle‐resolved electron energy loss spectroscopy. We found that the dispersion curve contains only the quadratic term. The vanishing of the linear term was ascribed to the presence in the film of Ag 5sp‐related quantum well states. Screening effects enhanced by electron confinement in Ag quantum well states push the position of the centroid of the induced charge of the surface plasmon less inside the interface compared to other Ag systems, rendering null the linear coefficient of the dispersion curve. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Design of Highly Sensitive Surface Plasmon Resonance Sensors Using Planar Metallic Films Closely Coupled to Nanogratings

We investigate the sensitivity enhancement of surface plasmon resonance （SPR） sensors using planar metallic films closely coupled to nanogratings. The strong coupling between localized surface plasmon resonances （LSPRs） presenting in metallic nanostructures and surface plasmon polaritons （SPPs） propagating at the metallic film surface leads to changes of resonance reflection properties, resulting in enhanced sensitivity of SPR sensors. The effects of thickness of the metallic films, grating period and metal materials on the refractive index sensitivity of the device are investigated. The refractive index sensitivity of nanograting-based SPR sensors is predicted to be about 543 nm/RIU （refractive index unit） using optimized structure parameters. Our study on SPR sensors using planar metallic films closely coupled to nanogratings demonstrates the potential for significant improvement in refractive index sensitivity.     

钼掺杂氧化锌薄膜的结构、光学和表面等离子体特性研究

室温下,通过直流磁控反应溅射在石英衬底上制备一系列钼掺杂氧化锌薄膜。分别采用X射线衍射(XRD)、原子力显微镜(AFM)、分光光度计及拉曼光谱仪研究了钼掺杂浓度对氧化锌薄膜结构、表面形貌、光学性能和表面等离子体特性的影响。XRD测试结果表明,零掺杂氧化锌薄膜结晶良好,呈c轴择优取向,掺杂后薄膜缺陷增多,结晶质量下降,当掺杂浓度达到3.93 Wt%时,薄膜由c轴择优取向的晶态转变为非晶态。AFM测试结果表明非晶态掺钼氧化锌薄膜表面光滑,粗糙度最低可达489 pm。透射光谱表明所有薄膜样品在可见光范围(400～760 nm)平均透过率均达到80%,禁带宽度随着掺杂浓度的提高从3.28 eV单调增加至3.60 eV。吸收光谱表明氧化锌薄膜表面等离子体共振吸收峰随钼掺杂量的增大发生蓝移,而拉曼光谱表明Mo重掺杂时ZnO薄膜表面拉曼散射信号强度显著降低。通过Mo掺杂获得非晶态氧化锌薄膜,拓宽了氧化锌薄膜材料的应用领域,同时研究了Mo掺杂浓度对氧化锌薄膜表面等离子体的调控作用,这对制备氧化锌基光子器件具有重要参考价值。     

Damping of the surface plasmon in clean and K-modified Ag thin films

The damping processes of electronic collective excitations of Ag/Ni(1 1 1) were studied by high-resolution electron energy spectroscopy. The FMHM of the Ag surface plasmon was reported as a function of Ag thickness, primary electron beam energy, Ag surface plasmon energy, and parallel momentum transfer. The broadening of the Ag surface plasmon was found to be related to 5sp–5sp transitions, for which a critical wave vector of 0.2 Å⁻¹ exists. Moreover, we provide a direct evidence of the occurrence of chemical interface damping in thin films, upon doping the Ag/Ni(1 1 1) system with K adatoms. The enhanced plasmon broadening in K/Ag/Ni(1 1 1) was ascribed to the existence of additional electron–hole decay channels at the K/Ag interface.     

氧化钛薄膜调控金属铜的表面等离子体共振特性研究

提出了一种利用氧化钛薄膜对金属铜薄膜表面等离子体共振特性调制的想法。实验中首先使用电子束蒸发制备一批同等厚度的氧化钛薄膜,再利用磁控溅射方法在氧化钛薄膜上沉积厚度为5～80 nm不等的金属铜薄膜。测试结果表明,氧化钛膜层对不同厚度的金属铜薄膜表面等离子体共振增强具有不同调制效果,金属铜薄膜厚度小于20 nm时,底层的氧化钛薄膜对Cu薄膜表面等离子体共振增强效果显著,且随着金属Cu膜层厚度增加表面等离子体共振峰发生蓝移,而当金属铜膜层的厚度超过20 nm时,共振增强效果因金属Cu薄膜消光能力的上升而开始减弱。     

Optical bistability of subwavelength metallic film coated by Kerr dielectric gratings

We studied the optical bistability of subwavelength metallic film coated by Kerr dielectric gratings numerically. It is found that the effect of optical bistability in the structure is explained by the excitations of the coupled surface plasmon polaritons at the coated metallic films. The effect of thickness of the metallic films on bistability loop is analyzed in detail, and the authors attribute the change of the bistability loop to the lifetime of the coupled surface plasmon polaritons.     

Propagation of THz plasmon pulse on corrugated and flat metal surface

We report here experiments on surface plasmon excitation and propagation along corrugated and smooth aluminum surface in the terahertz frequency range. Narrowband plasmon excitation by a subpicosecond terahertz pulse is shown to be a transient process and plasmon propagation sufficiently changes its measured time profile. Plasmon propagation during its excitation and detection changes measured signal. We suggest to use parameters T (plasmon duration) and τ (plasmon lifetime) to describe the narrowband THz plasmon pulse. Plasmon duration and lifetime were defined and plasmon propagation lengths on smooth and corrugated surface were measured. Plasmon propagation length on flat surface turned out to be much smaller than it is predicted by the Drude model.     

Plasmon energy chemical phase mapping of reactive multilayers

An analytical method of quantitative phase identification and mapping on the nanoscale is presented based on correlative similarity mapping from spectrum images within electron energy loss spectroscopy across the low‐loss plasmon region. The method is applied to map the reaction layer formation for heat treated Cu–Al–Al₂O₃ thin films. Coexistence of residual Al pockets next to polycrystalline but epitaxial CuAl₂ as main reaction product is found as well as a distinctive interfacial plasmon region. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Propagation oscillations in the near-field response of traveling surface waves launched by metallic nanoapertures

We discuss the implications of a frequency-dependent complex dielectric function ε(ω) of a metal for the interpretation of scanning near-field optical microscopy (SNOM) measurements in the vicinity of metallic nanoapertures. For subwavelength slits in gold films we observe distinct spatial intensity oscillations in the near-field signal for specific wavelengths in the visible spectrum. These oscillations of the SNOM signal far away from the nanoslit are ascribed to a constructive interference between the propagating surface plasmon (SP) with light scattered parallel to the gold–air interface. In these spatial SNOM-signal oscillations information about the surface plasmon dielectric function is encoded which can be extracted, for example, in surface plasmon interferometry for applications as sensors or waveguides.     

Formation of gold nanoparticles in heat-treated reactive co-sputtered Au-SiO2 thin films

In this work, formation of gold nanoparticles in radio frequency (RF) reactive magnetron co-sputtered Au-SiO₂ thin films post annealed at different temperatures in Ar + H₂ atmosphere has been investigated. Optical, surface topography, chemical state and crystalline properties of the prepared films were analyzed by using UV-visible spectrophotometry, atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS) and X-ray diffractometry (XRD) techniques, respectively. Optical absorption spectrum of the Au-SiO₂ thin films annealed at 800 °C showed one surface plasmon resonance (SPR) absorption peak located at 520 nm relating to gold nanoparticles. According to XPS analysis, it was found that the gold nanoparticles had a tendency to accumulate on surface of the heat-treated films in the metallic state. AFM images showed that the nanoparticles were uniformly distributed on the film surface with grain size of about 30 nm. Using XRD analysis average crystalline size of the Au particles was estimated to about 20 nm.     

银纳米颗粒对四苯基卟啉Q带荧光寿命的延长

文章报道了吸附在银纳米颗粒表面的四苯基卟啉(TPP)的Q带荧光寿命的变化.实验发现将银纳米颗粒的表面等离激元共振吸收峰调至与TPP的Q吸收带共振时,会使TPP的Q带荧光寿命得到延长.这是由于银纳米颗粒对表面的光电场有较大的表面等离激元共振增强效应,而处于激发态的TPP分子有较高的极性,这种增强的光电场会对有较高极性的TPP分子有稳定作用,所以延长了其Q带寿命.这对于以卟啉为光敏剂的光动力治疗有重要的意义.     

Collective excitations and quantum size effects on the surfaces of Pb(111) films: An experimental study

Pb(111) film is a special system that exhibits strong quantum size effects in many electronic properties. The collective excitations, i.e., plasmons, in Pb(111) films are also expected to show signatures of the quantum size effect. Here, using high-resolution electron energy loss spectroscopy, we measured the plasmons on the surface of Pb(111) films with different film thicknesses and analyzed the plasmon dispersions. One surface plasmon branch exhibits prominent damping in the small momentum range, which can be attributed to the interaction between the top and bottom interfaces of the Pb(111)films. With the film thickness increasing, the critical momentum characterizing the damping in Pb(111) films decays not only much slower in Pb(111) films than in other metal films, and even in films with the thickness up to 40 monolayers the damping still exists. The slow decay of the surface plasmon damping, manifesting the strong quantum size effect in Pb(111) films, might be related to the strong nesting of the Fermi surface along the(111) direction.     

Resonance and composition effects on the Raman scattering from silver-gold alloy clusters

Low-frequency Raman scattering experiments have been performed on thin films consisting of pure gold or gold-silver alloy clusters embedded in alumina matrix. It is clearly shown that the quadrupolar vibrational modes are observed by Raman scattering because of the effect of resonance with the excitation of the electronic surface dipolar plasmon. This is due to the strong coupling between the collective electronic dipolar excitation and the quadrupolar vibrational modes. This effect of resonance does not exist with the core electron excitations. The mixing of the conduction electron dipolar excitation (surface plasmon) with the core electrons leads to the quenching of the resonant Raman scattering. Received 16 November 2000     

Optical response of small-diameter semiconducting carbon nanotubes under exciton-surface-plasmon coupling

We analyze the optical response of small-diameter (?1 nm) semiconducting carbon nanotubes under the exciton-surface-plasmon coupling. Calculated optical absorption lineshapes exhibit the significant line (Rabi) splitting ∼0.1-0.3 eV as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube so that the mixed strongly coupled surface plasmon-exciton excitations are formed. We discuss possible ways to bring the exciton in resonance with the surface plasmon. The exciton-plasmon Rabi splitting effect we predict here for an individual carbon nanotube is close in its magnitude to that previously reported for hybrid plasmonic nanostructures artificially fabricated of organic semiconductors deposited on metallic films. We believe this effect may be used for the development of carbon nanotube based tunable optoelectronic device applications in areas such as nanophotonics and cavity quantum electrodynamics.     

Characterization of nanocrystalline gold/DLC composite films synthesized by plasma CVD technique

Composite films containing gold nanoparticles embedded in diamond-like carbon (Au-DLC) matrix were deposited on glass and Si (1 0 0) substrates by using capacitatively coupled plasma (CCP) chemical vapour deposition technique (CVD). Particle size and metal volume fraction were tailored by varying the relative amount of argon in the methane + argon gas mixture in the plasma. Optical constants of the films were evaluated. Bonding environment in these films were obtained from Raman and Fourier transformed infrared spectra (FTIR) studies. Blue-shift of the surface plasmon resonance peak in the optical absorbance spectra of the films could be associated with the reduction of the particle size while red shift was observed with the increase in volume fraction of metal particles in the DLC films. Absorption spectra recorded in the reflection mode indicated dichromatism in these films.     

Multilayer Au/TiO2Composite Films with Ultrafast Third-Order Nonlinear Optical Properties

We report on the ultrafast third-order optical nonlinearity in multilayer Au/TiO2 composite films fabricated on quartz substrates by pulsed laser deposition technique. The linear optical properties of the films are determined and optical absorption peaks due to surface plasmon resonance of Au particles are observed at about 590hm. The third-order optical nonlinearities of the films are investigated by z-scan method using a femtosecond laser （50 fs） at the wavelength of 800 nm. The sample showed fast nonlinear optical responses with nonlinear absorption coefficient and nonlinear refractive index being -3.66 × 10^-10 m/W and -2.95 × 10^-17 m^2/W, respectively. The results also show that the nonlinear optical effects increase with the increasing Au concentration in the composite films.     

Modifying Quantum Well States of Pb Thin Films via Interface Engineering

We demonstrate the importance of interface modification on improving electron confinement by preparing Pb quantum islands on Si（111） substrates with two different surface reconstructions, i.e., Si（111）-7 ×7 and Si（111）- Root3×Root3-Pb （hereafter, 7 ×7 and R3）. Characterization with scanning tunneling microscopy/spectroscopy shows that growing Pb films directly on a 7 × 7 surface will generate many interface defects, which makes the lifetime of quantum well states （QWSs） strongly dependent on surface locations. On the other hand, QWSs in Pb films on an R3 surface are well defined with small variations in linewidth on different surface locations and are much sharper than those on the 7 × 7 surface. We show that the enhancement in quantum confinement is primarily due to the reduced electron-defect scattering at the interface.     

Plasmonic tuning of aluminum doped zinc oxide nanostructures by atomic layer deposition

Currently there is a strong interest in plasmonic materials operating in the near‐infrared (NIR), however, conventional metals such as gold and silver possess high optical losses in this region. In this work we demonstrate localized surface plasmon resonances (LSPRs) with low loss in the NIR region by utilizing atomic layer deposition to deposit thin films of aluminium doped zinc oxide onto silicon nanopillars created via nanopshere lithography. The deposited films have excellent conformality and the LSPRs can be tuned from the mid‐infrared to the NIR by controlling the doping concentration, deposition temperature and nanostructure morphology. (© 2014 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Protecting TERS probes from degradation: extending mechanical and chemical stability

The detailed surface chemistry of aluminum oxide protected silver films for use specifically in surface enhanced Raman spectroscopy and tip enhanced Raman spectroscopy (TERS) was investigated. We have demonstrated that increased storage and scanning use lifetimes for silver plasmonic structures are directly connected with the elimination of chemical degradation at the plasmonic structure surface. X‐ray photoelectron spectroscopy of the metal films confirmed that a 2–3 nm thick coating of aluminum oxide prevented chemical attack of the underlying silver film for three months of storage in a desiccator, significantly increasing the storage lifetime of current probes. The scanning lifetime of a TERS probe when used to image a hard patterned silicon substrate was doubled with the addition of this protective coating. These measurements were performed without laser illumination in order to separate laser‐induced heating degradation from pure mechanical degradation of the metallized probe currently encountered during TERS data collection. Copyright © 2013 John Wiley & Sons, Ltd.