Label-free nanofluidic scattering microscopy of size and mass of single diffusing molecules and nanoparticles.

Label-free characterization of single biomolecules aims to complement fluorescence microscopy in situations where labeling compromises data interpretation, is technically challenging or even impossible. However, existing methods require the investigated species to bind to a surface to be visible, thereby leaving a large fraction of analytes undetected. Here, we present nanofluidic scattering microscopy (NSM), which overcomes these limitations by enabling label-free, real-time imaging of single biomolecules diffusing inside a nanofluidic channel. NSM facilitates accurate determination of molecular weight from the measured optical contrast and of the hydrodynamic radius from the measured diffusivity, from which information about the conformational state can be inferred. Furthermore, we demonstrate its applicability to the analysis of a complex biofluid, using conditioned cell culture medium containing extracellular vesicles as an example. We foresee the application of NSM to monitor conformational changes, aggregation and interactions of single biomolecules, and to analyze single-cell secretomes.

Light-driven transport of microparticles with phase-gradient metasurfaces.

Optical tweezers have opened numerous possibilities for precise control of microscopic particles for applications in life science and soft matter research and technology. However, traditional optical tweezers employ bulky conventional optics that prevents construction of compact optical manipulation systems. As an alternative, we present an ultrathin silicon-based metasurface that enables simultaneous confinement and propulsion of microparticles based on a combination of intensity and phase-gradient optical forces. The metasurface is constructed as a water-immersion line-focusing element that enables trapping and transport of 2µm particles over a wide area within a thin liquid cell. We envisage that the type of multifunctional metasurfaces reported herein will play a central role in miniaturized optical sensing, driving, and sorting of microscopic objects, such as cells or other biological entities.

Nanoscale Inorganic Motors Driven by Light: Principles, Realizations, and Opportunities.

The prospect of self-propelled artificial machines small enough to navigate within biological matter has fascinated and inspired researchers and the public alike since the dawn of nanotechnology. Despite many obstacles toward the realization of such devices, impressive progress on the development of its basic building block, the nanomotor, has been made over the past decade. Here, we review this emerging area with a focus on inorganic nanomotors driven or activated by light. We outline the distinct challenges and opportunities that differentiate nanomotors from micromotors based on a discussion of how stochastic forces influence the active motion of small particles. We introduce the relevant light-matter interactions and discuss how these can be utilized to classify nanomotors into three broad classes: nanomotors driven by optical momentum transfer, photothermal heating, and photocatalysis, respectively. On the basis of this classification, we then summarize and discuss the diverse body of nanomotor literature. We finally give a brief outlook on future challenges and possibilities in this rapidly evolving research area.

Protein kinase A controls yeast growth in visible light.

BACKGROUND: A wide variety of photosynthetic and non-photosynthetic species sense and respond to light, having developed protective mechanisms to adapt to damaging effects on DNA and proteins. While the biology of UV light-induced damage has been well studied, cellular responses to stress from visible light (400-700 nm) remain poorly understood despite being a regular part of the life cycle of many organisms. Here, we developed a high-throughput method for measuring growth under visible light stress and used it to screen for light sensitivity in the yeast gene deletion collection. RESULTS: We found genes involved in HOG pathway signaling, RNA polymerase II transcription, translation, diphthamide modifications of the translational elongation factor eEF2, and the oxidative stress response to be required for light resistance. Reduced nuclear localization of the transcription factor Msn2 and lower glycogen accumulation indicated higher protein kinase A (cAMP-dependent protein kinase, PKA) activity in many light-sensitive gene deletion strains. We therefore used an ectopic fluorescent PKA reporter and mutants with constitutively altered PKA activity to show that repression of PKA is essential for resistance to visible light. CONCLUSION: We conclude that yeast photobiology is multifaceted and that protein kinase A plays a key role in the ability of cells to grow upon visible light exposure. We propose that visible light impacts on the biology and evolution of many non-photosynthetic organisms and have practical implications for how organisms are studied in the laboratory, with or without illumination.

Optical Rotation and Thermometry of Laser Tweezed Silicon Nanorods.

Optical rotation of laser tweezed nanoparticles offers a convenient means for optical to mechanical force transduction and sensing at the nanoscale. Plasmonic nanoparticles are the benchmark system for such studies, but their rapid rotation comes at the price of high photoinduced heating due to Ohmic losses. We show that Mie resonant silicon nanorods with characteristic dimensions of ∼220 × 120 nm2 can be optically trapped and rotated at frequencies up to 2 kHz in water using circularly polarized laser light. The temperature excess due to heating from the trapping laser was estimated by phonon Raman scattering and particle rotation analysis. We find that the silicon nanorods exhibit slightly improved thermal characteristics compared to Au nanorods with similar rotation performance and optical resonance anisotropy. Altogether, the results indicate that silicon nanoparticles have the potential to become the system of choice for a wide range of optomechanical applications at the nanoscale.

Ultrafast Modulation of Thermoplasmonic Nanobubbles in Water.

Thermo-optically generated bubbles in water provide a powerful means for active matter control in microfluidic environments. These bubbles are often formed via continuous-wave illumination of an absorbing medium resulting in bubble nucleation via vaporization of water and subsequent bubble growth from the inward diffusion of gas molecules. However, to date, such bubbles tend to be several microns in diameter, resulting in slow dissipation. This limits the dynamic rate, spatial precision, and throughput of operation in any application. Here we show that isolated plasmonic structures can be utilized as highly localized heating elements to generate thermoplasmonic nanobubbles that can be modulated at frequencies up to several kilohertz in water, orders of magnitude faster than previously demonstrated for microbubbles. The nanobubbles are envisioned as advantageous localized active manipulation elements for high throughput microfluidic applications.

A Gaussian reflective metasurface for advanced wavefront manipulation.

Metasurfaces enable us to control the fundamental properties of light with unprecedented flexibility. However, most metasurfaces realized to date aim at modifying plane waves. While the manipulation of nonplanar wavefronts is encountered in a diverse number of applications, their control using metasurfaces is still in its infancy. Here we design a metareflector able to reflect a diverging Gaussian beam back onto itself with efficiency over 90% and focusing at an arbitrary distance. We outline a clear route towards the design of complex metareflectors that can find applications as diverse as optical tweezing, lasing, and quantum optics.

Solar harvesting based on perfect absorbing all-dielectric nanoresonators on a mirror.

The high-index all-dielectric nanoantenna system is a platform recently used for multiple applications, from metalenses to light management. These systems usually exhibit low absorption/scattering ratios and are not efficient photon harvesters. Nevertheless, by exploiting far-field interference, all-dielectric nanostructures can be engineered to achieve near-perfect absorption in specific wavelength ranges. Here, we propose - based on electrodynamics simulations - that a metasurface composed of an array of hydrogenated amorphous silicon nanoparticles on a mirror can achieve nearly complete light absorption close to the bandgap. We apply this concept to a realistic device, predicting a boost of optical performance of thin-film solar cells made of such nanostructures. In the proposed device, high-index dielectric nanoparticles act not only as nanoatennas able to concentrate light but also as the solar cell active medium, contacted at its top and bottom by transparent electrodes. By optimization of the exact geometrical parameters, we predict a system that could achieve initial conversion efficiency values well beyond 9% - using only the equivalent of a 75-nm thick active material. The device absorption enhancement is 50% compared to an unstructured device in the 400 nm - 550 nm range and more than 300% in the 650 nm - 700 nm spectral region. We demonstrate that such large values are related to the metasurface properties and to the perfect absorption mechanism.

Directional scattering and multipolar contributions to optical forces on silicon nanoparticles in focused laser beams.

Nanoparticles made of high index dielectric materials have seen a surge of interest and have been proposed for various applications, such as metalenses, light harvesting and directional scattering. With the advent of fabrication techniques enabling colloidal suspensions, the prospects of optical manipulation of such nanoparticles becomes paramount. High index nanoparticles support electric and magnetic multipolar responses in the visible regime and interference between such modes can give rise to highly directional scattering, in particular a cancellation of back-scattered radiation at the first Kerker condition. Here we present a study of the optical forces on silicon nanoparticles in the visible and near infrared calculated using the transfer matrix method. The zero-backscattering Kerker condition is investigated as an avenue to reduce radiation pressure in an optical trap. We find that while asymmetric scattering does reduce the radiation pressure, the main determining factor of trap stability is the increased particle response near the geometric resonances. The trap stability for non-spherical silicon nanoparticles is also investigated and we find that ellipsoidal deformation of spheres enables trapping of slightly larger particles.

Large-Scale Silicon Nanophotonic Metasurfaces with Polarization Independent Near-Perfect Absorption.

Optically thin perfect light absorbers could find many uses in science and technology. However, most physical realizations of perfect absorption for the optical range rely on plasmonic excitations in nanostructured metallic metasurfaces, for which the absorbed light energy is quickly lost as heat due to rapid plasmon decay. Here we show that a silicon metasurface excited in a total internal reflection configuration can absorb at least 97% of incident near-infrared light due to interferences between coherent electric and magnetic dipole scattering from the silicon nanopillars that build up the metasurface and the reflected wave from the supporting glass substrate. This "near-perfect" absorption phenomenon loads more than 50 times more light energy into the semiconductor than what would be the case for a uniform silicon sheet of equal surface density, irrespective of incident polarization. We envisage that the concept could be used for the development of novel light harvesting and optical sensor devices.

Wavevector-Selective Nonlinear Plasmonic Metasurfaces.

Electromagnetic metasurfaces with strong nonlinear responses and angular selectivity could offer many new avenues for designing ultrathin optics components. We investigated the optical second harmonic generation from plasmonic metasurfaces composed of aligned gold nanopillars with a pronounced out-of-plane tilt using a flexible nonlinear Fourier microscope. The experimental and computational results demonstrate that these samples function as wavevector-selective nonlinear metasurfaces, that is, the coherent second harmonic signal does not only depend on the polarization and wavelength of the excitation beam, but also of its direction of incidence, in spite of the subwavelength thickness of the active layer. Specifically, we observe that the nonlinear response can vary by almost two orders-of-magnitude when the incidence angle is changed from positive to negative values compared to the surface normal. Further, it is demonstrated that these metasurfaces act as a directional nonlinear mirrors, paving the way for new design of directional meta-mirrors in the nonlinear regime.

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.

Ultimate Limit of Light Extinction by Nanophotonic Structures.

Nanophotonic structures make it possible to precisely engineer the optical response at deep subwavelength scales. However, a fundamental understanding of the general performance limits remains a challenge. Here we use extensive electrodynamics simulations to demonstrate that the so-called f-sum rule sets a strict upper bound to the light extinction by nanostructures regardless their internal interactions and retardation effects. In particular, we show that the f-sum rule applies to arbitrarily complex plasmonic metal structures that exhibit an extraordinary spectral sensitivity to size, shape, near-field coupling effects, and incident polarization. The results may be used for benchmarking light scattering and absorption efficiencies, thus imposing fundamental limits on solar light harvesting, biomedical photonics, and optical communications.

Plasmon Enhanced Internal Photoemission in Antenna-Spacer-Mirror Based Au/TiO2 Nanostructures.

Emission of photoexcited hot electrons from plasmonic metal nanostructures to semiconductors is key to a number of proposed nanophotonics technologies for solar harvesting, water splitting, photocatalysis, and a variety of optical sensing and photodetector applications. Favorable materials and catalytic properties make systems based on gold and TiO2 particularly interesting, but the internal photoemission efficiency for visible light is low because of the wide bandgap of the semiconductor. We investigated the incident photon-to-electron conversion efficiency of thin TiO2 films decorated with Au nanodisk antennas in an electrochemical circuit and found that incorporation of a Au mirror beneath the semiconductor amplified the photoresponse for light with wavelength λ = 500-950 nm by a factor 2-10 compared to identical structures lacking the mirror component. Classical electrodynamics simulations showed that the enhancement effect is caused by a favorable interplay between localized surface plasmon excitations and cavity modes that together amplify the light absorption in the Au/TiO2 interface. The experimentally determined internal quantum efficiency for hot electron transfer decreases monotonically with wavelength, similar to the probability for interband excitations with energy higher than the Schottky barrier obtained from a density functional theory band structure simulation of a thin Au/TiO2 slab.

Realizing Strong Light-Matter Interactions between Single-Nanoparticle Plasmons and Molecular Excitons at Ambient Conditions.

Realizing strong light-matter interactions between individual two-level systems and resonating cavities in atomic and solid state systems opens up possibilities to study optical nonlinearities on a single-photon level, which can be useful for future quantum information processing networks. However, these efforts have been hampered by unfavorable experimental conditions, such as cryogenic temperatures and ultrahigh vacuum, required to study such systems and phenomena. Although several attempts to realize strong light-matter interactions at room temperature using plasmon resonances have been made, successful realizations on the single-nanoparticle level are still lacking. Here, we demonstrate the strong coupling between plasmons confined within a single silver nanoprism and excitons in molecular J aggregates at ambient conditions. Our findings show that deep subwavelength mode volumes V together with quality factors Q that are reasonably high for plasmonic nanostructures result in a strong-coupling figure of merit-Q/sqrt[V] as high as ∼6×10^{3} µm^{-3/2}, a value comparable to state-of-the-art photonic crystal and microring resonator cavities. This suggests that plasmonic nanocavities, and specifically silver nanoprisms, can be used for room temperature quantum optics.

A thermal plasmonic sensor platform: resistive heating of nanohole arrays.

We have created a simple and efficient thermal plasmonic sensor platform by letting a DC current heat plasmonic nanohole arrays. The sensor can be used to determine thermodynamic parameters in addition to monitoring molecular reactions in real-time. As an application example, we use the thermal sensor to determine the kinetics and activation energy for desorption of thiol monolayers on gold. Further, the temperature of the metal can be measured optically by the spectral shift of the bonding surface plasmon mode (0.015 nm/K). We show that this resonance shift is caused by thermal lattice expansion, which reduces the plasma frequency of the metal. The sensor is also used to determine the thin film thermal expansion coefficient through a theoretical model for the expected resonance shift.

Plasmonic particles set into fast orbital motion by an optical vortex beam.

We optically trap plasmonic gold particles in two dimensions and set them into circular motion around the optical axis using a helically phased vortex laser beam. The orbiting frequency of the particles reaches 86 Hz, which corresponds to a particle velocity of the order 1 mm per second, for an incident laser power of a few tens of milliwatts. The experimentally determined orbiting frequencies are found to be well in line with the notion that the beam carries an orbital angular momentum of hl per photon.

Complete light annihilation in an ultrathin layer of gold nanoparticles.

We experimentally demonstrate that an incident light beam can be completely annihilated in a single layer of randomly distributed, widely spaced gold nanoparticle antennas. Under certain conditions, each antenna dissipates more than 10 times the number of photons that enter its geometric cross-sectional area. The underlying physics can be understood in terms of a critical coupling to localized plasmons in the nanoparticles or, equivalently, in terms of destructive optical Fano interference and so-called coherent absorption.

Ultrafast spinning of gold nanoparticles in water using circularly polarized light.

Controlling the position and movement of small objects with light is an appealing way to manipulate delicate samples, such as living cells or nanoparticles. It is well-known that optical gradient and radiation pressure forces caused by a focused laser beam enables trapping and manipulation of objects with strength that is dependent on the particle's optical properties. Furthermore, by utilizing transfer of photon spin angular momentum, it is also possible to set objects into rotational motion simply by targeting them with a beam of circularly polarized light. Here we show that this effect can set ∼200 nm radii gold particles trapped in water in 2D by a laser tweezers into rotation at frequencies that reach several kilohertz, much higher than any previously reported light driven rotation of a microscopic object. We derive a theory for the fluctuations in light scattering from a rotating particle, and we argue that the high rotation frequencies observed experimentally is the combined result of favorable optical particle properties and a low local viscosity due to substantial heating of the particles surface layer. The high rotation speed suggests possible applications in nanofluidics, optical sensing, and microtooling of soft matter.

Synchronization of optically self-assembled nanorotors.

Self-assembly of nanoparticles by means of interparticle optical forces provides a compelling approach toward contact-free organization and manipulation of nanoscale entities. However, exploration of the rotational degrees of freedom in this process has remained limited, primarily because of the predominant focus on spherical nanoparticles, for which individual particle orientation cannot be determined. Here, we show that gold nanorods, which self-assemble in water under the influence of circularly polarized light, exhibit synchronized rotational motion at kilohertz frequencies. The synchronization is caused by strong optical interactions and occurs despite the presence of thermal diffusion. Our findings elucidate the intricate dynamics arising from the transfer of photon spin angular momentum to optically bound matter and hold promise for advancing the emerging field of light-driven nanomachinery.