Lei Shao

Gold Nanorod Rotary Motors Driven by Resonant Light Scattering.

Efficient and robust artificial nanomotors could provide a variety of exciting possibilities for applications in physics, biology and chemistry, including nanoelectromechanical systems, biochemical sensing, and drug delivery. However, the application of current man-made nanomotors is limited by their sophisticated fabrication techniques, low mechanical output power and severe environmental requirements, making their performance far below that of natural biomotors. Here we show that single-crystal gold nanorods can be rotated extremely fast in aqueous solutions through optical torques dominated by plasmonic resonant scattering of circularly polarized laser light with power as low as a few mW. The nanorods are trapped in 2D against a glass surface, and their rotational dynamics is highly dependent on their surface plasmon resonance properties. They can be kept continuously rotating for hours with limited photothermal side effects and they can be applied for detection of molecular binding with high sensitivity. Because of their biocompatibility, mechanical and thermal stability, and record rotation speeds reaching up to 42 kHz (2.5 million revolutions per minute), these rotary nanomotors could advance technologies to meet a wide range of future nanomechanical and biomedical needs in fields such as nanorobotics, nanosurgery, DNA manipulation and nano/microfluidic flow control.

Hot Electron Generation and Cathodoluminescence Nanoscopy of Chiral Split Ring Resonators

Three-dimensional chiral plasmonic nanostructures have been shown to be able to dramatically boost photon-spin selective light-matter interactions, potentially leading to novel photonics, molecular spectroscopy, and light-harvesting applications based on circularly polarized light. Here, we show that chiral split-ring gold nanoresonators interfaced to a wide band gap semiconductor exhibit a contrast in hot-electron transfer rate between left-handed and right-handed visible light that essentially mimics the far-field circular dichroism of the structures. We trace down the origin of this effect to the differential excitation of the thinnest part of the split-ring structures using dichroic-sensitive cathodoluminescence imaging with nanometer spatial resolution. The results highlight the intricate interplay between the near-field and far-field chiral response of a nanostructure and establishes a clear link to the emerging field of hot carrier plasmonics with numerous potential applications in photocatalysis and solar light harvesting.

Plasmonic Metasurfaces with Conjugated Polymers for Flexible Electronic Paper in Color

A flexible electronic paper in full color is realized by plasmonic metasurfaces with conjugated polymers. An ultrathin large-area electrochromic material is presented which provides high polarization-independent reflection, strong contrast, fast response time, and long-term stability. This technology opens up for new electronic readers and posters with ultralow power consumption.

Continuous-Gradient Plasmonic Nanostructures Fabricated by Evaporation on a Partially Exposed Rotating Substrate.

A continuous-gradient approach of material evaporation is employed to fabricate nanostructures with varying geometric parameters, such as thickness, lateral positioning, and orientation on a single substrate. The method developed for mask lithography allows continuous tuning of the physical properties of a sample. The technique is highly valuable in simplifying the overall optimization process for constructing metasurfaces.

Brownian fluctuations of an optically rotated nanorod

Gold nanorods can be optically trapped in aqueous solution and forced to rotate at kilohertz rates by circularly polarized laser light. This enables detailed investigations of local environmental p ...

Metasurfaces and Colloidal Suspensions Composed of 3D Chiral Si Nanoresonators

High-refractive-index silicon nanoresonators are promising low-loss alternatives to plasmonic particles in CMOS-compatible nanophotonics applications. However, complex 3D particle morphologies are challenging to realize in practice, thus limiting the range of achievable optical functionalities. Using 3D film structuring and a novel gradient mask transfer technique, the first intrinsically chiral dielectric metasurface is fabricated in the form of a monolayer of twisted silicon nanocrescents that can be easily detached and dissolved into colloidal suspension. The metasurfaces exhibit selective handedness and a circular dichroism as large as 160° µm-1 due to pronounced differences in induced current loops for left-handed and right-handed polarization. The detailed morphology of the detached particles is analyzed using high-resolution transmission electron microscopy. Furthermore, it is shown that the particles can be manipulated in solution using optical tweezers. The fabrication and detachment method can be extended to different nanoparticle geometries and paves the way for a wide range of novel nanophotonic experiments and applications of high-index dielectrics.

Probing Photothermal Effects on Optically Trapped Gold Nanorods by Simultaneous Plasmon Spectroscopy and Brownian Dynamics Analysis

Plasmonic gold nanorods are prime candidates for a variety of biomedical, spectroscopy, data storage, and sensing applications. It was recently shown that gold nanorods optically trapped by a focused circularly polarized laser beam can function as extremely efficient nanoscopic rotary motors. The system holds promise for applications ranging from nanofluidic flow control and nanorobotics to biomolecular actuation and analysis. However, to fully exploit this potential, one needs to be able to control and understand heating effects associated with laser trapping. We investigated photothermal heating of individual rotating gold nanorods by simultaneously probing their localized surface plasmon resonance spectrum and rotational Brownian dynamics over extended periods of time. The data reveal an extremely slow nanoparticle reshaping process, involving migration of the order of a few hundred atoms per minute, for moderate laser powers and a trapping wavelength close to plasmon resonance. The plasmon spectroscopy and Brownian analysis allows for separate temperature estimates based on the refractive index and the viscosity of the water surrounding a trapped nanorod. We show that both measurements yield similar effective temperatures, which correspond to the actual temperature at a distance of the order 10-15 nm from the particle surface. Our results shed light on photothermal processes on the nanoscale and will be useful in evaluating the applicability and performance of nanorod motors and optically heated nanoparticles for a variety of applications.

Optically controlled stochastic jumps of individual gold nanorod rotary motors

Brownian microparticles diffusing in optical potential-energy landscapes constitute a generic test bed for nonequilibrium statistical thermodynamics and have been used to emulate a wide variety of physical systems, ranging from Josephson junctions to Carnot engines. Here we demonstrate that it is possible to scale down this approach to nanometric length scales by constructing a tilted washboard potential for the rotation of plasmonic gold nanorods. The potential depth and tilt can be precisely adjusted by modulating the light polarization. This allo`ws for a gradual transition from continuous rotation to discrete stochastic jumps, which are found to follow Kramers dynamics in excellent agreement with stochastic simulations. The results widen the possibilities for fundamental experiments in statistical physics and provide insights into how to construct light-driven nanomachines and multifunctional sensing elements.

Antibody-Antigen Interaction Dynamics Revealed by Analysis of Single-Molecule Equilibrium Fluctuations on Individual Plasmonic Nanoparticle Biosensors

Antibody-antigen interactions are complex events central to immune response, in vivo and in vitro diagnostics, and development of therapeutic substances. We developed an ultrastable single-molecule localized surface plasmon resonance (LSPR) sensing platform optimized for studying antibody-antigen interaction kinetics over very long time scales. The setup allowed us to perform equilibrium fluctuations analysis of the PEG/anti-PEG interaction. By time and frequency domain analysis, we demonstrate that reversible adsorption of monovalently bound anti-PEG antibodies is the dominant factor affecting the LSPR fluctuations. The results suggest that equilibrium fluctuation analysis can be an alternative to established methods for determination of interaction rates. In particular, the methodology is suited to analyze molecular systems whose properties change during the initial interaction phases, for example, due to mass transport limitations or, as demonstrated here, because the effective association rate constant varies with surface concentration of adsorbed molecules.

Fabrication of continuous gradient plasmonic nanostructures

Metallic nanostructures constitute one of the most important building blocks of contemporary nanoscience and nanotechnology because they support localized surface plasmon resonances (LSPRs) that dramatically enhance light-matter interactions. However, LSPRs are strongly dependent on nanostructure sizes, shapes, orientations and interparticle distances. The plasmonic properties of individual metal nanostructures therefore need to be finely tuned by optimizing their geometrical parameters. Conventional techniques, including both bottom-up wet-chemistry growth and top-down lithography, are not perfect and manufacturing uncertainties can result in considerable deviations from the desired optical behaviour. The preparation of specific structures therefore often requires sequential optimization processes that are repetitive, time consuming and costly.