Nanophotonic force microscopy: characterizing particle-surface interactions using near-field photonics.

Direct measurements of particle-surface interactions are important for characterizing the stability and behavior of colloidal and nanoparticle suspensions. Current techniques are limited in their ability to measure pico-Newton scale interaction forces on submicrometer particles due to signal detection limits and thermal noise. Here we present a new technique for making measurements in this regime, which we refer to as nanophotonic force microscopy. Using a photonic crystal resonator, we generate a strongly localized region of exponentially decaying, near-field light that allows us to confine small particles close to a surface. From the statistical distribution of the light intensity scattered by the particle we are able to map out the potential well of the trap and directly quantify the repulsive force between the nanoparticle and the surface. As shown in this Letter, our technique is not limited by thermal noise, and therefore, we are able to resolve interaction forces smaller than 1 pN on dielectric particles as small as 100 nm in diameter.

Near-field Light Scattering Techniques for Measuring Nanoparticle-Surface Interaction Energies and Forces.

Nanoparticles are quickly becoming commonplace in many commercial and industrial products, ranging from cosmetics to pharmaceuticals to medical diagnostics. Predicting the stability of the engineered nanoparticles within these products a priori remains an important and difficult challenge. Here we describe our techniques for measuring the mechanical interactions between nanoparticles and surfaces using near-field light scattering. Particle-surface interfacial forces are measured by optically "pushing" a particle against a reference surface and observing its motion using scattered near-field light. Unlike atomic force microscopy, this technique is not limited by thermal noise, but instead takes advantage of it. The integrated waveguide and microfluidic architecture allow for high-throughput measurements of about 1000 particles per hour. We characterize the reproducibility of and experimental uncertainty in the measurements made using the NanoTweezer surface instrument. We report surface interaction studies on gold nanoparticles with 50 nm diameters, smaller than previously reported in the literature using similar techniques.

HI-Light: A Glass-Waveguide-Based "Shell-and-Tube" Photothermal Reactor Platform for Converting CO2 to Fuels.

In this work, we introduce HI-Light, a surface-engineered glass-waveguide-based "shell-and-tube" type photothermal reactor which is both scalable in diameter and length. We examine the effect of temperature, light irradiation, and residence time on its photo-thermocatalytic performance for CO2 hydrogenation to form CO, with a cubic phase defect-laden indium oxide, In2O3-x(OH)y, catalyst. We demonstrate the light enhancement effect under a variety of reaction conditions. Notably, the light-on performance for the cubic nanocrystal photocatalyst exhibits a CO evolution rate at 15.40 mmol gcat -1 hr-1 at 300°C and atmospheric pressure. This is 20 times higher conversion rate per unit catalyst mass per unit time beyond previously reported In2O3-x(OH)y catalyst in the cubic form under comparable operation conditions and more than 5 times higher than that of its rhombohedral polymorph. This result underscores that improvement in photo-thermocatalytic reactor design enables uniform light distribution and better reactant/catalyst mixing, thus significantly improving catalyst utilization.

Simultaneous Characterization of Nanoparticle Size and Particle-Surface Interactions with Three-Dimensional Nanophotonic Force Microscopy.

The behavior of a nanoparticle in solution depends strongly on the particle's physical and chemical characteristics, most notably the particle size and the surface properties. Accurately characterizing these properties is critical for quality control in a wide variety of industries. To understand a complex and polydisperse nanoparticle suspension, however, ensemble averaging is not sufficient, and there is a great need for direct measurements of size and surface properties at the individual nanoparticle level. In this work, we present an analysis technique for simultaneous characterization of particle-surface interactions and size using near-field light scattering and verify it using Brownian-dynamics simulations. Using a nanophotonic waveguide, single particles can be stably held near the waveguide's surface by strongly localized optical forces. By tracking the dynamic 3D motion of the particle under the influence of these forces using an optical microscope, it is possible to extract the particle-surface interaction forces, as well as to estimate the size and refractive index of the nanoparticle. Because of the strong light-scattering signal, this method is viable for high-throughput characterization of particles as small as 100 nm in only a few seconds each.

Dynamics of an optically confined nanoparticle diffusing normal to a surface.

Here we measure the hindered diffusion of an optically confined nanoparticle in the direction normal to a surface, and we use this to determine the particle-surface interaction profile in terms of the absolute height. These studies are performed using the evanescent field of an optically excited single-mode silicon nitride waveguide, where the particle is confined in a height-dependent potential energy well generated from the balance of optical gradient and surface forces. Using a high-speed cmos camera, we demonstrate the ability to capture the short time-scale diffusion dominated motion for 800-nm-diam polystyrene particles, with measurement times of only a few seconds per particle. Using established theory, we show how this information can be used to estimate the equilibrium separation of the particle from the surface. As this measurement can be made simultaneously with equilibrium statistical mechanical measurements of the particle-surface interaction energy landscape, we demonstrate the ability to determine these in terms of the absolute rather than relative separation height. This enables the comparison of potential energy landscapes of particle-surface interactions measured under different experimental conditions, enhancing the utility of this technique.

Nanophotonic detection of freely interacting molecules on a single influenza virus.

Biomolecular interactions, such as antibody-antigen binding, are fundamental to many biological processes. At present, most techniques for analyzing these interactions require immobilizing one or both of the interacting molecules on an assay plate or a sensor surface. This is convenient experimentally but can constrain the natural binding affinity and capacity of the molecules, resulting in data that can deviate from the natural free-solution behavior. Here we demonstrate a label-free method for analyzing free-solution interactions between a single influenza virus and specific antibodies at the single particle level using near-field optical trapping and light-scattering techniques. We determine the number of specific antibodies binding to an optically trapped influenza virus by analyzing the change of the Brownian fluctuations of the virus. We develop an analytical model that determines the increased size of the virus resulting from antibodies binding to the virus membrane with uncertainty of ± 1-2 nm. We present stoichiometric results of 26 ± 4 (6.8 ± 1.1 attogram) anti-influenza antibodies binding to an H1N1 influenza virus. Our technique can be applied to a wide range of molecular interactions because the nanophotonic tweezer can handle molecules from tens to thousands of nanometers in diameter.