Plasmas meet plasmonics

The term ‘plasmon’ was first coined in 1956 to describe collective electronic oscillations in solids which were very similar to electronic oscillations/surface waves in a plasma discharge (effectively the same formulae can be used to describe the frequencies of these physical phenomena). Surface waves originating in a plasma were initially considered to be just a tool for basic research, until they were successfully used for the generation of large-area plasmas for nanoscale materials synthesis and processing. To demonstrate the synergies between ‘plasmons’ and ‘plasmas’, these large-area plasmas can be used to make plasmonic nanostructures which functionally enhance a range of emerging devices. The incorporation of plasma-fabricated metal-based nanostructures into plasmonic devices is the missing link needed to bridge not only surface waves from traditional plasma physics and surface plasmons from optics, but also, more topically, macroscopic gaseous and nanoscale metal plasmas. This article first presents a brief review of surface waves and surface plasmons, then describe how these areas of research may be linked through Plasma Nanoscience showing, by closely looking at the essential physics as well as current and future applications, how everything old, is new, once again.

Enhancement of optical absorption in thin-film solar cells through the excitation of higher-order nanoparticle plasmon modes

Recent research in the rapidly emerging field of plasmonics has shown the potential to significantly enhance light trapping inside thin-film solar cells by using metallic nanoparticles. In this article it is demonstrated the plasmon enhancement of optical absorption in amorphous silicon solar cells by using silver nanoparticles. Based on the analysis of the higher-order surface plasmon modes, it is shown how spectral positions of the surface plasmons affect the plasmonic enhancement of thin-film solar cells. By using the predictive 3D modeling, we investigate the effect of the higher-order modes on that enhancement. Finally, we suggest how to maximize the light trapping and optical absorption in the thin-film cell by optimizing the nanoparticle array parameters, which in turn can be used to fine tune the corresponding surface plasmon modes.

Binding mechanism of affinity ligands for purification of plasmid DNA

Plasmid DNA for therapeutic and vaccination purposes must be highly purified. The high selectivity of affinity chromatography makes it ideal for the isolation of pDNA from complex biological feed stocks. Affinity chromatography makes use of the biological function and/or individual chemical structure of the interacting molecules. However, the success of any affinity purification protocol is dependent on the availability of suitable ligands. In this study, surface plasmon resonance (SPR) based Biacore system has been employed for the detection and quantification of the binding between lac operon (lacO) sequence contained in a pDNA and synthetic peptides based on the DNA-binding domain of the lac repressor protein, lad. The equilibrium dissociation constant (K D) and association and dissociation rate constants (ka, kd) for the interaction between plasmid DNA and designed peptides were determined.

Mechanisms of ultrafast laser-induced deep-subwavelength gratings on graphite and diamond

Deep-subwavelength gratings with periodicities of 170, 120, and 70 nm can be observed on highly oriented pyrolytic graphite irradiated by a femtosecond (fs) laser at 800 nm. Under picosecond laser irradiation, such gratings likewise can be produced. Interestingly, the 170-nm grating is also observed on single-crystal diamond irradiated by the 800-nm fs laser. In our opinion, the optical properties of the high-excited state of material surface play a key role for the formation of the deep-subwavelength gratings. The numerical simulations of the graphite deep-subwavelength grating at normal and high-excited states confirm that in the groove the light intensity can be extraordinarily enhanced via cavity-mode excitation in the condition of transverse-magnetic wave irradiation with near-ablation-threshold fluences. This field enhancement of polarization sensitiveness in deep-subwavelength apertures acts as an important feedback mechanism for the growth and polarization dependence of the deep-subwavelength gratings. In addition, we suggest that surface plasmons are responsible for the formation of seed deep-subwavelength apertures with a particular periodicity and the initial polarization dependence. Finally, we propose that the nanoscale Coulomb explosion occurring in the groove is responsible for the ultrafast nonthermal ablation mechanism.

Light-matter Interactions in Semiconductors and Metals: From Nitride Optoelectronics to Quantum Plasmonics

This thesis puts forth a theory-directed approach coupled with spectroscopy aimed at the discovery and understanding of light-matter interactions in semiconductors and metals.

The first part of the thesis presents the discovery and development of Zn-IV nitride materials.The commercial prominence in the optoelectronics industry of tunable semiconductor alloy materials based on nitride semiconductor devices, specifically InGaN, motivates the search for earth-abundant alternatives for use in efficient, high-quality optoelectronic devices. II-IV-N2 compounds, which are closely related to the wurtzite-structured III-N semiconductors, have similar electronic and optical properties to InGaN namely direct band gaps, high quantum efficiencies and large optical absorption coefficients. The choice of different group II and group IV elements provides chemical diversity that can be exploited to tune the structural and electronic properties through the series of alloys. The first theoretical and experimental investigation of the ZnSnxGe1−xN2 series as a replacement for III-nitrides is discussed here.

The second half of the thesis shows ab−initio calculations for surface plasmons and plasmonic hot carrier dynamics. Surface plasmons, electromagnetic modes confined to the surface of a conductor-dielectric interface, have sparked renewed interest because of their quantum nature and their broad range of applications. The decay of surface plasmons is usually a detriment in the field of plasmonics, but the possibility to capture the energy normally lost to heat would open new opportunities in photon sensors, energy conversion devices and switching. A theoretical understanding of plasmon-driven hot carrier generation and relaxation dynamics in the ultrafast regime is presented here. Additionally calculations for plasmon-mediated upconversion as well as an energy-dependent transport model for these non-equilibrium carriers are shown.

Finally, this thesis gives an outlook on the potential of non-equilibrium phenomena in metals and semiconductors for future light-based technologies.

Classical and Quantum Effects in Plasmonic Metals

The field of plasmonics exploits the unique optical properties of metallic nanostructures to concentrate and manipulate light at subwavelength length scales. Metallic nanostructures get their unique properties from their ability to support surface plasmons– coherent wave-like oscillations of the free electrons at the interface between a conductive and dielectric medium. Recent advancements in the ability to fabricate metallic nanostructures with subwavelength length scales have created new possibilities in technology and research in a broad range of applications.

In the first part of this thesis, we present two investigations of the relationship between the charge state and optical state of plasmonic metal nanoparticles. Using experimental bias-dependent extinction measurements, we derive a potential- dependent dielectric function for Au nanoparticles that accounts for changes in the physical properties due to an applied bias that contribute to the optical extinction. We also present theory and experiment for the reverse effect– the manipulation of the carrier density of Au nanoparticles via controlled optical excitation. This plasmoelectric effect takes advantage of the strong resonant properties of plasmonic materials and the relationship between charge state and optical properties to eluci- date a new avenue for conversion of optical power to electrical potential.

The second topic of this thesis is the non-radiative decay of plasmons to a hot-carrier distribution, and the distribution’s subsequent relaxation. We present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. We also preform ab initio calculations of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We extend these first-principle methods to calculate the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions. Finally, we combine these first-principles calculations of carrier dynamics and optical response to produce a complete theoretical description of ultrafast pump-probe measurements, free of any fitting parameters that are typical in previous analyses.

On the dynamic readout of sub-diffraction-limit pit arrays with a silver thin film

Fast moving arrays of periodic sub-diffraction-limit pits were dynamically read out via a silver thin film. The mechanism of the dynamic readout is analysed and discussed in detail, both experimentally and theoretically. The analysis and experiment show that, in the course of readout, surface plasmons can be excited at the silver/air interface by the focused laser beam and amplified by the silver thin film. The surface plasmons are transmitted into the substrate/silver interface with a large enhancement. The surface waves at the substrate/silver interface are scattered by the sinusoidal pits of sub-diffraction-limit size. The scattered waves are collected by a converging lens and guided into the detector for the readout.

Subwavelength plasmonics for graded-index optics on a chip.

Planar plasmonic devices are becoming attractive for myriad applications, owing to their potential compatibility with standard microelectronics technology and the capability for densely integrating a large variety of plasmonic devices on a chip. Mitigating the challenges of using plasmonics in on-chip configurations requires precise control over the properties of plasmonic modes, in particular their shape and size. Here we achieve this goal by demonstrating a planar plasmonic graded-index lens focusing surface plasmons propagating along the device. The plasmonic mode is manipulated by carving subwavelength features into a dielectric layer positioned on top of a uniform metal film, allowing the local effective index of the plasmonic mode to be controlled using a single binary lithographic step. Focusing and divergence of surface plasmons is demonstrated experimentally. The demonstrated approach can be used for manipulating the propagation of surface plasmons, e.g., for beam steering, splitting, cloaking, mode matching, and beam shaping applications.

Plasmonic nanofocusing of light in an integrated silicon photonics platform.

The capability to focus electromagnetic energy at the nanoscale plays an important role in nanoscinece and nanotechnology. It allows enhancing light matter interactions at the nanoscale with applications related to nonlinear optics, light emission and light detection. It may also be used for enhancing resolution in microscopy, lithography and optical storage systems. Hereby we propose and experimentally demonstrate the nanoscale focusing of surface plasmons by constructing an integrated plasmonic/photonic on chip nanofocusing device in silicon platform. The device was tested directly by measuring the optical intensity along it using a near-field microscope. We found an order of magnitude enhancement of the intensity at the tip's apex. The spot size is estimated to be 50 nm. The demonstrated device may be used as a building block for "lab on a chip" systems and for enhancing light matter interactions at the apex of the tip.

Plasmonic nanotips for on-chip nanoscale confinement of light

We demonstrate the on-chip nanoscale focusing of surface plasmons in metallic nanotip coupled to the silicon waveguide. Strong field enhancement is observed at the apex of the tip. Enhancing light matter interactions is discussed. © 2012 OSA.

Plasmonic nanotips for on-chip nanoscale confinement of light

We demonstrate the on-chip nanoscale focusing of surface plasmons in metallic nanotip coupled to the silicon waveguide. Strong field enhancement is observed at the apex of the tip. Enhancing light matter interactions is discussed. © 2011 Optical Society of America.

Simulation of light coupling enhancement and localization of transmission field via subwavelength metallic gratings

Surface plasmons(SPs) generated in nano metallic gratings on medium layer can greatly enhance the transmission field through the metallic gratings. The enhancement effect is achieved from lambda = 500 nm to near-infrared domain. The enhancement rate is about 110 % at the wavelength of about 6 10 nm and about 180 % at lambda = 700 nm and 740 nm where most kinds of thin film solar cells have a high spectral response. These structures should provide a promising way to increase the coupling efficiency of thin film solar cells and optical detectors of different wavelength response.

Quantifying the effectiveness of SiO2/Au light trapping nanoshells for thin film poly-Si solar cells

In order to enhance light absorption of thin film poly-crystalline silicon (TF poly-Si) solar cells over a broad spectral range, and quantify the effectiveness of nanoshell light trapping structure over the full solar spectrum in theory, the effective photon trapping flux (EPTF) and effective photon trapping efficiency (EPTE) were firstly proposed by considering both the external quantum efficiency of TF poly-Si solar cell and scattering properties of light trapping structures. The EPTF, EPTE and scattering spectrum exhibit different behaviors depending on the geometric size and density of nanoshells that form the light trapping layer. With an optimum size and density of SiO2/Au nanoshell light trapping layer, the EPTE could reach up to 40% due to the enhancement of light trapping over a broad spectral range, especially from 500 to 800 nm.

亚波长金属光栅的光耦合增强效应及透射局域化的模拟研究

介质层上的亚波长金属光栅产生的表面等离子体(surface plasmons,SPs)可以极大地增强光栅下介质层内的透射光强.增强作用从500 nm延续到近红外区域.在波长610 nm附近有接近110%的增强,在波长700 nm及740nm处也有180%左右的增强.而这个波长范围与薄膜太阳能电池的吸收谱很相近,因此这种结构有望大幅度提高薄膜太阳能电池及不同波长光探测嚣等光电转换器件的光耦合效率.

Design of Fluorescent Assays for Cyanide and Hydrogen Peroxide Based on the Inner Filter Effect of Metal Nanoparticles

We have demonstrated the design of a new type fluorescent assay based on the inner filter effect (IFE) of metal nanoparticles (NPs), which is conceptually different from the previously reported metal NPs-based fluorescent assays. With a high extinction coefficient and tunable plasmon absorption feature, metal NPs are expected to be capable of functioning as a powerful absorber to tune the emission of the fluorophore in the IFE-based fluorescent assays. In this work, we presented two proof-of-concept examples based on the IFE of Au NPs by choosing MDMO-PPV as a model fluorophore, whose fluorescence could be tuned by the absorbance of Au NPs with a much higher sensitivity than the corresponding absorbance approach.