As science progresses at the nanoscopic level, it becomes more and more important to comprehend the interactions taking place at the nanoscale, where optical near-fields play a key role. Their phenomenology differs significantly from the propagative light we experience at the macroscopic level. This is particularly important in applications such as surface-enhanced spectroscopies for single-molecule detection, where often the optimization of the plasmonic structures and surfaces relies on far-field characterizations. The processes dominating in the far-field picture, though, are not the same dominating in the near-field. To highlight this, we resort to very simple metallic systems: Isolated gold nanorods in solution. We show how single-walled nanotubes can be exploited to read out processes occurring at the near-field level around metallic nanoparticles and make the information accessible in the far-field region. This is implemented by monitoring the spectral profile of the enhancement of the photoluminescence and Raman signal of the nanotubes for several excitation wavelengths. Through this excitation-resolved study, we show that the far-field optical read-out detects the transversal and longitudinal dipolar plasmonic oscillations of gold nanorods, whereas the near-field read-out through the nanotubes reveals other mechanisms to dominate. The spectral position of the maximum enhancement of the optical near-field mediated signals are located elsewhere than the far-field bands. This dichotomy between near-field and far-field response should be taken into account when optimizing plasmonic nanostructures for applications such as surface-enhanced spectroscopies.
We study the refractive-index sensing properties of plasmonic nanotubes with a dielectric core and ultra-thin metal shell. The few-nm thin metal shell is described by both the usual Drude model and the nonlocal hydrodynamic model to investigate the effects of nonlocality. We derive an analytical expression for the extinction cross section and show how sensing of the refractive index of the surrounding medium and the figure-of-merit are affected by the shape and size of the nanotubes. Comparison with other localized surface plasmon resonance sensors reveals that the nanotube exhibits superior s…
Investigating the cellular internalization pathways of single molecules or single nano-objects is important to understanding cell-matter interactions and to applications in drug delivery and discovery. Imaging and tracking the motion of single molecules on cell plasma membrane require high spatial resolution in three dimensions (3D). Fluorescence imaging along the axial dimension with nanometer resolution has been highly challenging but critical to revealing displacements in trans-membrane events. Here, utilizing a plasmonic ruler based on the sensitive distance dependence of near-infrared flu…
We present an analytical model describing complex dynamics of a hybrid nonlinear system consisting of interacting carbon nanotubes (CNT) and a plasmonic metamaterial. Our model is based on the set of coupled equations, which incorporates well-established density matrix formalism appropriate for quantum systems (CNT are described as a two level system) and harmonic-oscillator approach ideal for modelling sub-wavelength plasmonic and optical resonators. We show that the saturation nonlinearity of CNT increases multifold in the resonantly enhanced near field of a metamaterial. In the framework of…
Metallic nanoparticle-on-a-mirror (NPoM) cavities enable extreme field confinement in sub-nm gaps, leading to unrivaled performance for nonlinear processes such as surface-enhanced Raman scattering (SERS). So far, prevailing experimental approaches based on NPoMs have been performed by means of free-space light excitation and collection under oblique incidence, since the fundamental radiatively-coupled NPoM mode does not scatter in the normal direction. Retaining this working principle, here we numerically show that plasmonic cavity modes in NPoM configurations can be efficiently excited in an…
Carbon nanotubes provide a rare access point into the plasmon physics of one-dimensional electronic systems. By assembling purified nanotubes into uniformly sized arrays, we show that they support coherent plasmon resonances, that these plasmons enhance and hybridize with phonons, and that the phonon-plasmon resonances have quality factors as high as 10. Because coherent nanotube plasmonics can strengthen light-matter interactions, it provides a compelling platform for surface-enhanced infrared spectroscopy and tunable, high-performance optical devices at the nanometer scale.
Nanotubes of various kinds have been prepared in the last decade, starting from the discovery of carbon nanotubes. Recently other types of nanotubes including metallic (Au), inorganic (TiO2, HfS2, V7O16, CdSe, MoS2), and polymeric (polyaniline, polyacrylonitrile) have been produced. Herein we present a novel synthetic procedure leading to a new kind of porous, high-surface-area nanoparticle nanotubes (NPNTs). This study characterizes the synthesized silver nanotubes at optical wavelengths. The absorption spectrum of PAN washed silver nanotubes shows an extended absorption peak at visible wavel…
Nitrogen vacancy (NV) centers in diamond have emerged as a leading quantum sensor platform, combining exceptional sensitivity with nanoscale spatial resolution by optically detected magnetic resonance (ODMR). Because fluorescence-based ODMR techniques are limited by low photon collection efficiency and modulation contrast, there has been growing interest in infrared (IR)-absorption-based readout of the NV singlet state transition. IR readout can improve contrast and collection efficiency, but it has thus far been limited to long-pathlength geometries in bulk samples due to the small absorption…
Graphene is a unique material to study fundamental limits of plasmonics. Apart from the ultimate single-layer thickness, its carrier concentration can be tuned by chemical doping or applying an electric field. In this manner the electrodynamic properties of graphene can be varied from highly conductive to dielectric. Graphene supports strongly confined, propagating surface plasmon-polaritons (SPPs) in a broad spectral range from terahertz to mid-infrared frequencies. It also possesses a strong magneto-optical response and thus provides complimentary architectures to conventional magneto-plasmo…
Highly-anisotropic plasmonic nanotubes exhibit a dramatic drop of the scattering cross section in the transition regime from hyperbolic to elliptic dispersion. The characterization of a realistic multilayered metamaterial is typically carried out by means of an effective medium approach providing average components of the permittivity tensor and wave fields. Here, the edge effects of the metal-dielectric stratified nanotube for different combinations were thoroughly analyzed. We show how the boundary layers, which in principle remain fully irrelevant in the estimation of the effective permitti…
Metamaterials, artificial media structured on the subwavelength scale offer a rich paradigm for developing unique photonic functionalities ranging from negative index of refraction and directionally asymmetric transmission to slowing light. Here we demonstrate that a combination of carbon nanotubes with a photonic metamaterial offers a new paradigm for the development of nonlinear media with exceptionally strong ultrafast nonlinear response invaluable in photonic applications. It is underpinned by strong coupling between weakly radiating Fano-type resonant plasmonic modes and the excitonic res…
While long-range propagating plasmons have been extensively investigated for implementing on-chip optical sensing platforms, waveguide-excited localized surface plasmon resonance (LSPR) based sensing systems have not yet received much attention. Waveguide excitation and readout as an alternative to free-space light based single-particle spectroscopy are particularly attractive for high-throughput sensing and on-chip drug discovery platforms. Here we present a numerical investigation of the optical response of a waveguide-excited plasmonic dolmen-shaped compound nanoantenna that exhibits a Fano…
Low-dimensional plasmonic materials can function as high quality terahertz and infrared antennas at deep subwavelength scales. Despite these antennas' strong coupling to electromagnetic fields, there is a pressing need to further strengthen their absorption. We address this problem by fabricating thick films of aligned, uniformly sized carbon nanotubes and showing that their plasmon resonances are strong, narrow, and broadly tunable. With thicknesses ranging from 25 to 250 nm, our films exhibit peak attenuation reaching 70%, quality factors reaching 9, and electrostatically tunable peak freque…
Long wave infrared detection using probabilistic spintronic bolometer arrays
Elmore Family School of Electrical and Computer Engineering, Purdue University（普渡大学埃尔莫电气与计算机工程学院）；Department of Physics and Astronomy, Purdue University（普渡大学物理与天文系）；Department of Materials Engineering, Indian Institute of Science（印度科学学院材料工程系）
We explain the Lorentz resonances in plasmonic crystals that consist of 2D nano dielectric inclusions as the interaction between resonant material properties and geometric resonances of electrostatic nature. One example of such plasmonic crystals are graphene nanosheets that are periodically arranged within a non-magnetic bulk dielectric. We identify local geometric resonances on the length scale of the small scale period. From a materials perspective, the graphene surface exhibits a dispersive surface conductance captured by the Drude model. Together these phenomena conspire to generate Loren…
Optical nanosensors are promising for hydrogen sensing because they are small, free from spark generation, and feasible for remote optical readout. Conventional optical nanosensors require broadband excitation and spectrometers, rendering the devices bulky and complex. An alternative is spatial intensity-based optical sensing, which only requires an imaging system and a smartly designed platform to report the spatial distribution of analytical optical signals. Here, we present a spatial intensity-based hydrogen sensing platform based on Fano-like spatial distribution of the transmission in a P…
Graphene plasmons are rapidly emerging as a viable tool for fast electrical manipulation of light. The prospects for applications to electro-optical modulation, optical sensing, quantum plasmonics, light harvesting, spectral photometry, and tunable lighting at the nanoscale are further stimulated by the relatively low level of losses and high degree of spatial confinement that characterize these excitations compared with conventional plasmonic materials. We start with a general description of the plasmons in extended graphene, followed by analytical methods that lead to reasonably accurate est…
Recent years have seen an explosive research and development of nanoplasmonics in the visible and near-infrared (near-ir) frequency regions. One of the most fundamental effects in nanoplasmonics is nano-concentration of optical energy. Plasmonic nanofocusing has been predicted and experimentally achieved. It will be very beneficial for the fundamental science, engineering, environmental, and defense applications to be able to nano-concentrate terahertz radiation (frequency 1 - 10 THz or vacuum wavelength 300 - 30 microns). This will allow for the nanoscale spatial resolution for THz imaging an…
Physical property of a single quantum object is governed by its precise atomic arrangement. The direct correlation of localized physical properties with the atomic structures has been therefore strongly desired but still limited in the theoretical studies. Here, we have successfully examined the localized electronic properties of individual carbon nanotubes by means of high-resolution electron energy-loss spectroscopy combined with high-resolution transmission electron microscopy. Well-separated sharp peaks at the carbon K(1s) absorption edge and in the valence-loss spectra are obtained from a…
