Resonant dielectric multilayer with controlled absorption for enhanced total internal reflection fluorescence microscopy.

Total internal reflection fluorescence microscopy (TIRF-M) is widely used in biological imaging. Evanescent waves, generated at the glass-sample interface, theoretically strongly improve the axial resolution down to a hundred of nanometers. However, objective based TIRF-M suffers from different limitations such as interference fringes and uneven illumination, mixing both propagating and evanescent waves, which degrade the image quality. In principle, uneven illumination could be avoided by increasing the excitation angle, but this results in a drastic loss of excitation power. We designed dedicated 1D photonic crystals in order to circumvent this power loss by directly acting on the intensity of the evanescent field at controlled incident angles. In this framework, we used dedicated resonant multi-dielectric stacks, supporting Bloch surface waves and resulting in large field enhancement when illuminated under the conditions of total internal reflection. Here, we present a numerical optimization of such resonant stacks by adapting the resulting resonance to the angular illumination conditions in TIRF-M and to the fluorescence collection constraints. We thus propose a dedicated resonant structure with a control of the absorption during thin film deposition. A first experimental demonstration illustrates the concept with a 3-fold fluorescence enhancement in agreement with the numerical predictions.

Sensitivity of resonance properties of all-dielectric multilayers driven by statistical fluctuations.

In photonics and emerging fields of quantum and topological materials, increasing demands are placed upon the state and control of electromagnetic fields. Dielectric multilayer materials may be designed and optimized to possess extremely sharp spectral and angular photonic resonances allowing for the creation of fields orders of magnitude larger than the exciting field. With enhancements of 104 and higher, the extreme nature of these resonances places high constraints on the statistical properties of the physical and optical characteristics of the materials. To what extent the spectral and angular shifts occur as a result of fluctuations in the refractive indices and morphologies of the involved low-loss subdomains have not been considered previously. Here, we present how parameter variations such as those caused by fluctuations in deposition rate, yielding bias, random and compensated errors, may affect the resonance properties of low-loss all-dielectric stacks.

Bandwidths limitations of giant optical field enhancements in dielectric multi-layers.

Dielectric multilayers, when properly optimized, have been shown to sustain giant optical field enhancement directly linked to the imaginary index of the materials. Such giant optical field is of great interests to increase tremendously the sensitivity of optoelectronic systems. Unfortunately, this ultra-sensitive system is also highly depending on the illumination conditions. We discuss here the effect of the angular divergence and the spectral bandwidth of the incident laser beam on the absorption and field enhancement. In this study, we clearly show that giant optical field enhancements, up to several decades, may be achievable when the incident conditions are down few µrad and pm in term of angular and spectral bandwidths respectively.

Plasmon assisted thermal modulation in nanoparticles.

Single-particle interactions hold the promise of nanometer-scale devices in areas such as data communications and storage, nanolithography, waveguides, renewable energy and therapeutics. We propose that the collective electronic properties possessed by noble metal nanoparticles may be exploited for device actuation via the unapparent mechanism of plasmon-assisted heat generation and flux. The temperature dependence of the dielectric function and the thermal transport properties of the particles play the central role in the feasibility of the thermally-actuated system, however the behavior of these thermoplasmonic processes is unclear. We experimentally and computationally analyzed modulation via thermoplasmonic processes on a test system of gold (Au) nano-islands. Modulation and energy transport in discontinuous domains exhibited quantitatively different characteristics compared to thin films. The results have implications for all surface plasmon based nano-devices where inevitable small-scale thermal processes are present.

Spectroscopy and imaging of arrays of nanorods toward nanopolarimetry.

The polarization dependence of the optical scattering properties of two-dimensional arrays of metal nanostructures with sub-wavelength dimensions (nanoantennas) has been investigated. Arrays of 500 nm × 100 nm gold nanorods covering a 100 × 100 µm(2) area were fabricated with varying orientations on an electrically conductive substrate. The experimental and computational analysis of the angularly organized nanorods suggest potential use toward the development of an integrated polarimeter. Using the gold nanorods on a transparent substrate as a preliminary system, we show that in the proper spectral range the scattering properties of the structures may be tuned for such an application.

Discontinuity induced angular distribution of photon plasmon coupling.

Metal-dielectric transitions are important structures that can display a host of optical characteristics including excitation of plasmons. Metal-dielectric discontinuities can furthermore support plasmon excitation without a severe condition on the incident angle of the exciting photons. Using a semi-infinite thin gold film, we study surface plasmon (SP) excitation and the associated electromagnetic near-field distribution by recording the resulting plasmon interference patterns. In particular, we measure interference periods involving SPs at the scanable metal/air interface and the buried metal/glass one. Supported by optical near-field simulations and experiments, we demonstrate that the metal/glass surface plasmon is observable over a wide range of incident angles encompassing values above and below the critical incident angle. As a result, it is shown that scanning near-field microscopy can provide quantitative evaluation of the real part of the buried surface plasmon wavevector.

Nanometrology of delignified Populus using mode synthesizing atomic force microscopy.

The study of the spatially resolved physical and compositional properties of materials at the nanoscale is increasingly challenging due to the level of complexity of biological specimens such as those of interest in bioenergy production. Mode synthesizing atomic force microscopy (MSAFM) has emerged as a promising metrology tool for such studies. It is shown that, by tuning the mechanical excitation of the probe-sample system, MSAFM can be used to dynamically investigate the multifaceted complexity of plant cells. The results are argued to be of importance both for the characteristics of the invoked synthesized modes and for accessing new features of the samples. As a specific system to investigate, we present images of Populus, before and after a holopulping treatment, a crucial step in the biomass delignification process.

Laser reflectometry of submegahertz liquid meniscus ringing.

Optical techniques that permit nondestructive probing of interfacial dynamics of various media are of key importance in numerous applications such as ellipsometry, mirage effect, and all-optical switching. Characterization of the various phases of microjet droplet formation yields important information for volume control, uniformity, velocity, and rate. The ringing of the meniscus and the associated relaxation time that occurs after droplet breakoff affect subsequent drop formation and is an indicator of the physical properties of the fluid. Using laser reflectometry, we present an analysis of the meniscus oscillations in an orifice of a piezoelectric microjet.

Individual gold dimers investigated by far- and near-field imaging.

Plasmon resonances in 3D nanoparticle arrangements can produce strong localized optical fields, which are of importance for any application involving interaction of light with subwavelength volumes of matter down to the molecular level. In particular, remarkable field enhancement and confinement occur in a dimer geometry formed by two identical closely spaced particles. Although, recent advances in nanofabrication have rendered the fabrication of complex plasmon architectures more accessible, addressing their local fields in a nonperturbative fashion remains not straightforward, because metallic nanostructures are rather sensitive to their local environment. Here we study gold dimers fabricated by e-beam lithography. Individual dimers are imaged both by far- and near-field methods. First, the near-field electromagnetic interaction in an ensemble of dimers is investigated by scattering spectroscopy, using dark field microscopy. Next, to probe their local field, we explore the luminescence of individual gold dimers utilizing a confocal microscope with single molecule detection sensitivity. We provide a statistical analysis of the dimer luminescence for different incident polarizations, with direct comparison to single particles (monomers). Finally, the near-field transmission of the resonant dimers is mapped with a subwavelength resolution using polarized controlled near-field scanning optical microscopy. Surprisingly, no clear evidence of the high mode density in the dimer gap is observed. This result may be attributed to the limited coupling of the field emitted by the aperture probe to the dimer mode.

An experimental investigation of analog delay generation for dynamic control of microsensors and atomic force microscopy.

We present an implementation of pure-time-delay generation in analog signals located in the kilo-Hertz frequency band. The controlled constant delays that are produced engage in a feedback system to investigate the dynamic response of microcantilevers. Delayed systems offer a vast richness of eigenvalues resulting in the possibility of excitations at frequencies other than that of the fundamental mode. Different cantilever actuation and delay generation approaches are investigated and compared, and detailed experimental observation of the dynamic response of the system is presented. Based on our results, an acoustic excitation is devised that may be used as an efficient sensor.

Plasticity, elasticity, and adhesion energy of plant cell walls: nanometrology of lignin loss using atomic force microscopy.

The complex organic polymer, lignin, abundant in plants, prevents the efficient extraction of sugars from the cell walls that is required for large scale biofuel production. Because lignin removal is crucial in overcoming this challenge, the question of how the nanoscale properties of the plant cell ultrastructure correlate with delignification processes is important. Here, we report how distinct molecular domains can be identified and how physical quantities of adhesion energy, elasticity, and plasticity undergo changes, and whether such quantitative observations can be used to characterize delignification. By chemically processing biomass, and employing nanometrology, the various stages of lignin removal are shown to be distinguished through the observed morphochemical and nanomechanical variations. Such spatially resolved correlations between chemistry and nanomechanics during deconstruction not only provide a better understanding of the cell wall architecture but also is vital for devising optimum chemical treatments.

Microscale Marangoni actuation: all-optical and all-electrical methods.

We present experimental results from an all-optical microfluidic platform that may be complimented by a thin film all-electrical network. Using these configurations we have studied the microfluidic convective flow systems of silicone oil, glycerol, and 1,3,5-trinitrotoluene on open surfaces through the production of surface tension gradients derived from thermal gradients. We show that sufficient localized thermal variation can be created utilizing surface plasmons and/or engaging individually addressable resistive thermal elements. Both studies manipulate fluids via Marangoni forces, each having their unique exploitable advantages. Surface plasmon excitation in metal foils are the driving engine of many physical-, chemical-, and bio-sensing applications. Incorporating, for the first time, the plasmon concept in microfluidics, our results thus demonstrate great potential for simultaneous fluid actuation and sensing.

Nonradiative surface plasmon assisted microscale Marangoni forces.

When a liquid droplet experiences a temperature inhomogeneity along its bounding surface, a surface energy gradient is engendered, which when, in a continuous sense, exceeding a threshold, results in a convective flow dissipating the energy. If the associated temperature gradients are sustained by the interface between the liquid and a supporting substrate, the induced flow can result in the lateral motion of the droplet overcoming the viscosity and inertia. Recently, pico-liter adsorbed and applied droplets were shown experimentally to be transported, and divided by the decay of optically excited surface plasmons into phonons in a thin gold foil. The decaying events locally modify the temperature of the liquid-solid interface, establishing microscale thermal gradients of sufficient magnitude for the droplet to undergo thermocapillary flow. We present experimental evidence of such gradients resulting in local surface modification associated with the excitation of surface plasmons. We show theoretically that the observed effect is due to Marangoni forces, and computationally visualize the flow characteristics for the experimental parameters. As an application based on our results, we propose a method for an all-optical modulation of light by light mediated by the droplet oscillations. Furthermore, the results have important consequences for microfluidics, droplet actuation, and simultaneous surface plasmon resonance sensing and spectroscopy.

Probing large area surface plasmon interference in thin metal films using photon scanning tunneling microscopy.

The interference of surface plasmons can provide important information regarding the surface features of the hosting thin metal film. We present an investigation of the interference of optically excited surface plasmons in the Kretschmann configuration in the visible spectrum. Large area surface plasmon interference regions are generated at several wavelengths and imaged with the photon scanning tunneling microscope. Furthermore, we discuss the non-retarded dispersion relations for the surface plasmons in the probe-metal system modeled as confocal hyperboloids of revolution in the spheroidal coordinate systems.

Modulation of multiple photon energies by use of surface plasmons.

A form of optical modulation at low pulse rates is reported in the case of surface plasmons excited by 1.55-microm photons in a thin gold foil. Several visible-photon energies are shown to be pulsed by the action of the infrared pulses, the effect being maximized when each visible beam also excites surface plasmons. The infrared surface plasmons are implicated as the primary cause of thermally induced changes in the foil. The thermal effects dissipate in sufficiently small times so that operation up to the kilohertz range in pulse repetition frequency is obtained. Unlike direct photothermal phenomena, no phase change is necessary for the effect to be observed.