Femtosecond Drift Photocurrents Generated by an Inversely Designed Plasmonic Antenna.

Photocurrents play a crucial role in various applications, including light detection, photovoltaics, and THz radiation generation. Despite the abundance of methods and materials for converting light into electrical signals, the use of metals in this context has been relatively limited. Nanostructures supporting surface plasmons in metals offer precise light manipulation and induce light-driven electron motion. Through the inverse design optimization of a gold nanostructure, we demonstrate enhanced volumetric, unidirectional, intense, and ultrafast photocurrents via a magneto-optical process derived from the inverse Faraday effect. This is achieved through fine-tuning the amplitude, polarization, and gradients in the local light field. The virtually instantaneous process allows dynamic photocurrent modulation by varying optical pulse duration, potentially yielding nanosources of intense, ultrafast, planar magnetic fields and frequency-tunable THz emission. These findings open avenues for ultrafast magnetic material manipulation and hold promise for nanoscale THz spectroscopy.

Broadband Plasmonic Nanoantennas for Multi-Color Nanoscale Dynamics in Living Cells.

Recently, the implementation of plasmonic nanoantennas has opened new possibilities to investigate the nanoscale dynamics of individual biomolecules in living cells. However, studies so far have been restricted to single molecular species as the narrow wavelength resonance of gold-based nanostructures precludes the simultaneous interrogation of different fluorescently labeled molecules. Here, broadband aluminum-based nanoantennas carved at the apex of near-field probes are exploited to resolve nanoscale-dynamic molecular interactions on living cell membranes. Through multicolor excitation, the authors simultaneously recorded fluorescence fluctuations of dual-color labeled transmembrane receptors known to form nanoclusters. Fluorescence cross-correlation studies revealed transient interactions between individual receptors in regions of ≈60 nm. Moreover, the high signal-to-background ratio provided by the antenna illumination allowed the authors to directly detect fluorescent bursts arising from the passage of individual receptors underneath the antenna. Remarkably, by reducing the illumination volume below the characteristic receptor nanocluster sizes, the molecular diffusion within nanoclusters is resolved and distinguished from nanocluster diffusion. Spatiotemporal characterization of transient interactions between molecules is crucial to understand how they communicate with each other to regulate cell function. This work demonstrates the potential of broadband photonic antennas to study multi-molecular events and interactions in living cell membranes with unprecedented spatiotemporal resolution.

Exploring the Magnetic and Electric Side of Light through Plasmonic Nanocavities.

Light-matter interactions are often considered to be mediated by the electric component of light only, neglecting the magnetic contribution. However, the electromagnetic energy density is equally distributed between both parts of the optical fields. Within this scope, we experimentally demonstrate here, in excellent agreement with numerical simulations, that plasmonic nanostructures can selectively manipulate and tune the magnetic versus electric emission of luminescent nanocrystals. In particular, we show selective enhancement or decay of magnetic and electric emission from trivalent europium-doped nanoparticles in the vicinity of plasmonic nanocavities, designed to efficiently couple to either the electric or magnetic emission of the quantum emitter. Specifically, by precisely controlling the spatial position of the emitter with respect to our plasmonic nanostructures, by means of a near-field optical microscope, we record local distributions of both magnetic and electric radiative local densities of states (LDOS) with nanoscale precision. The distribution of the radiative LDOS reveals the modification of both the magnetic and electric optical quantum environments induced by the presence of the metallic nanocavities. This manipulation and enhancement of magnetic light-matter interaction by means of plasmonic nanostructures opens up new possibilities for the research fields of optoelectronics, chiral optics, nonlinear and nano-optics, spintronics, and metamaterials, among others.

Enhancing Magnetic Light Emission with All-Dielectric Optical Nanoantennas.

Electric and magnetic optical fields carry the same amount of energy. Nevertheless, the efficiency with which matter interacts with electric optical fields is commonly accepted to be at least 4 orders of magnitude higher than with magnetic optical fields. Here, we experimentally demonstrate that properly designed photonic nanoantennas can selectively manipulate the magnetic versus electric emission of luminescent nanocrystals. In particular, we show selective enhancement of magnetic emission from trivalent europium-doped nanoparticles in the vicinity of a nanoantenna tailored to exhibit a magnetic resonance. Specifically, by controlling the spatial coupling between emitters and an individual nanoresonator located at the edge of a near-field optical scanning tip, we record with nanoscale precision local distributions of both magnetic and electric radiative local densities of states (LDOS). The map of the radiative LDOS reveals the modification of both the magnetic and electric quantum environments induced by the presence of the nanoantenna. This manipulation and enhancement of magnetic light-matter interaction by means of nanoantennas opens up new possibilities for the research fields of optoelectronics, chiral optics, nonlinear and nano-optics, spintronics, and metamaterials, among others.

Doubly Resonant Photonic Antenna for Single Infrared Quantum Dot Imaging at Telecommunication Wavelengths.

Colloidal quantum dots (CQDs) have drawn strong interest in the past for their high prospects in scientific, medical, and industrial applications. However, the full characterization of these quantum emitters is currently restricted to the visible wavelengths, and it remains a key challenge to optically probe single CQDs operating in the infrared spectral domain, which is targeted by a growing number of applications. Here, we report the first experimental detection and imaging at room temperature of single infrared CQDs operating at telecommunication wavelengths. Imaging was done with a doubly resonant bowtie nanoaperture antenna (BNA) written at the end of a fiber nanoprobe, whose resonances spectrally fit the CQD absorption and emission wavelengths. Direct near-field characterization of PbS CQDs reveal individual nanocrystals with a spatial resolution of 75 nm (λ/20) together with their intrinsic 2D dipolar free-space emission properties and exciton dynamics (blinking phenomenon). Because the doubly resonant BNA is strongly transmissive at both the CQD absorption and the emission wavelengths, we are able to perform all-fiber nanoimaging with a standard 20% efficiency InGaAs avalanche photodiode (APD). The detection efficiency is predicted to be 3000 fold larger than with a conventional circular aperture tip of the same transmission area. Double resonance BNA fiber probes thus offer the possibility of exploring extreme light-matter interaction in low band gap CQDs with current plug-and-play detection techniques, opening up new avenues in the fields of infrared light-emitting devices, photodetectors, telecommunications, bioimaging, and quantum information technology.

Plasmonic Nanoantennas Enable Forbidden Förster Dipole-Dipole Energy Transfer and Enhance the FRET Efficiency.

Förster resonance energy transfer (FRET) plays a key role in biochemistry, organic photovoltaics, and lighting sources. FRET is commonly used as a nanoruler for the short (nanometer) distance between donor and acceptor dyes, yet FRET is equally sensitive to the mutual dipole orientation. The orientation dependence complicates the FRET analysis in biological samples and may even lead to the absence of FRET for perpendicularly oriented donor and acceptor dipoles. Here, we exploit the strongly inhomogeneous and localized fields in plasmonic nanoantennas to open new energy transfer routes, overcoming the limitations from the mutual dipole orientation to ultimately enhance the FRET efficiency. We demonstrate that the simultaneous presence of perpendicular near-field components in the nanoantenna sets favorable energy transfer routes that increase the FRET efficiency up to 50% for nearly perpendicular donor and acceptor dipoles. This new facet of plasmonic nanoantennas enables dipole-dipole energy transfer that would otherwise be forbidden in a homogeneous environment. As such, our approach further increases the applicability of single-molecule FRET over diffraction-limited approaches, with the additional benefits of higher sensitivities and higher concentration ranges toward physiological levels.

All-Dielectric Silicon Nanogap Antennas To Enhance the Fluorescence of Single Molecules.

Plasmonic antennas have a profound impact on nanophotonics as they provide efficient means to manipulate light and enhance light-matter interactions at the nanoscale. However, the large absorption losses found in metals can severely limit the plasmonic applications in the visible spectral range. Here, we demonstrate the effectiveness of an alternative approach using all-dielectric nanoantennas based on silicon dimers to enhance the fluorescence detection of single molecules. The silicon antenna design is optimized to confine the near-field intensity in the 20 nm nanogap and reach a 270-fold fluorescence enhancement in a nanoscale volume of λ(3)/1800 with dielectric materials only. Our conclusions are assessed by combining polarization resolved optical spectroscopy of individual antennas, scanning electron microscopy, numerical simulations, fluorescence lifetime measurements, fluorescence burst analysis, and fluorescence correlation spectroscopy. This work demonstrates that all-silicon nanoantennas are a valid alternative to plasmonic devices for enhanced single molecule fluorescence sensing, with the additional key advantages of reduced nonradiative quenching, negligible heat generation, cost-efficiency, and complementary metal-oxide-semiconductor (CMOS) compatibility.

Large-Scale Arrays of Bowtie Nanoaperture Antennas for Nanoscale Dynamics in Living Cell Membranes.

We present a novel blurring-free stencil lithography patterning technique for high-throughput fabrication of large-scale arrays of nanoaperture optical antennas. The approach relies on dry etching through nanostencils to achieve reproducible and uniform control of nanoantenna geometries at the nanoscale, over millimeter-sizes in a thin aluminum film. We demonstrate the fabrication of over 400 000 bowtie nanoaperture (BNA) antennas on biocompatible substrates, having gap sizes ranging from (80 ± 5) nm down to (20 ± 10) nm. To validate their applicability on live cell research, we used the antenna substrates as hotspots of localized illumination to excite fluorescently labeled lipids on living cell membranes. The high signal-to-background afforded by the BNA arrays allowed the recording of single fluorescent bursts corresponding to the passage of freely diffusing individual lipids through hotspot excitation regions as small as 20 nm. Statistical analysis of burst length and intensity together with simulations demonstrate that the measured signals arise from the ultraconfined excitation region of the antennas. Because these inexpensive antenna arrays are fully biocompatible and amenable to their integration in most fluorescence microscopes, we foresee a large number of applications including the investigation of the plasma membrane of living cells with nanoscale resolution at endogenous expression levels.

Matching Nanoantenna Field Confinement to FRET Distances Enhances Förster Energy Transfer Rates.

Förster resonance energy transfer (FRET) is widely applied in chemistry, biology, and nanosciences to assess distances on sub-10 nm scale. Extending the range and applicability of FRET requires enhancement of the fluorescence energy transfer at a spatial scale comparable to the donor-acceptor distances. Plasmonic nanoantennas are ideal to concentrate optical fields at a nanoscale fully matching the FRET distance range. Here, we present a resonant aluminum nanogap antenna tailored to enhance single molecule FRET. A 20 nm gap confines light into a nanoscale volume, providing a field gradient on the scale of the donor-acceptor distance, a large 10-fold increase in the local density of optical states, and strong intensity enhancement. With our dedicated design, we obtain 20-fold enhancement on the fluorescence emission of donor and acceptor dyes, and most importantly up to 5-fold enhancement of the FRET rate for donor-acceptor separations of 10 nm. We also provide a thorough framework of the fluorescence photophysics occurring in the nanoscale gap volume. The presented enhancement of energy transfer flow at the nanoscale opens a yet unexplored facet of the various advantages of optical nanoantennas and provides a new strategy toward biological applications of single molecule FRET at micromolar concentrations.

Hybrid photonic antennas for subnanometer multicolor localization and nanoimaging of single molecules.

Photonic antennas amplify and confine optical fields at the nanoscale offering excellent perspectives for nanoimaging and nanospectroscopy. Increased resolution beyond the diffraction limit has been demonstrated using a variety of antenna designs, but multicolor nanoscale imaging is precluded by their resonance behavior. Here we report on the design of a novel hybrid antenna probe based on a monopole nanoantenna engineered on a bowtie nanoaperture. The device combines broadband enhanced emission, extreme field confinement down to few nanometers, and zero-background illumination. We demonstrate simultaneous dual-color single molecule nanoimaging with 20 nm resolution and angstrom localization precision, corresponding to 10(3)-fold improvement compared to diffraction-limited optics. When interacting with individual molecules in the near-field, our innovative design enables the emission of 10(4) photon-counts per molecule in a 20 nm excitation region, allowing direct discrimination of spectrally distinct molecules separated by 2.1 ± 0.4 nm. We foresee that background-free nanolight sources will open new horizons in optical nanoscopy and fluorescence spectroscopy by providing multicolor detection of standard fluorescent molecules fully compatible with live cell research.

Light funneling from a photonic crystal laser cavity to a nano-antenna: overcoming the diffraction limit in optical energy transfer down to the nanoscale.

We show that the near-field coupling between a photonic crystal microlaser and a nano-antenna can enable hybrid photonic systems that are both physically compact (free from bulky optics) and efficient at transferring optical energy into the nano-antenna. Up to 19% of the laser power from a micron-scale photonic crystal laser cavity is experimentally transferred to a bowtie aperture nano-antenna (BNA) whose area is 400-fold smaller than the overall emission area of the microlaser. Instead of a direct deposition of the nano-antenna onto the photonic crystal, it is fabricated at the apex of a fiber tip to be accurately placed in the microlaser near-field. Such light funneling within a hybrid structure provides a path for overcoming the diffraction limit in optical energy transfer to the nanoscale and should thus open promising avenues in the nanoscale enhancement and confinement of light in compact architectures, impacting applications such as biosensing, optical trapping, local heating, spectroscopy, and nanoimaging.

Ultrabright bowtie nanoaperture antenna probes studied by single molecule fluorescence.

We report on a novel design for the fabrication of ultrabright bowtie nanoaperture antenna (BNA) probes to breach the intrinsic trade-off between power transmission and field confinement of circular nanoapertures as in near-field scanning optical microscopy (NSOM) or planar zero mode waveguides. The approach relies on the nanofabrication of BNAs at the apex of tapered optical fibers tuned to diameters close to their cutoff region, resulting in 10(3)× total improvement in throughput over conventional NSOM probes of similar confinement area. By using individual fluorescence molecules as optical nanosensors, we show for the first time nanoimaging of single molecules using BNA probes with an optical confinement of 80 nm, measured the 3D near-field emanating from these nanostructures and determined a ~6-fold enhancement on the single molecule signal. The broadband field enhancement, nanoscale confinement, and background free illumination provided by these nanostructures offer excellent perspectives as ultrabright optical nanosources for a full range of applications, including cellular nanoimaging, spectroscopy, and biosensing.

Tesla-Range Femtosecond Pulses of Stationary Magnetic Field, Optically Generated at the Nanoscale in a Plasmonic Antenna.

The inverse Faraday effect allows the generation of stationary magnetic fields through optical excitation only. This light-matter interaction in metals results from creating drift currents via nonlinear forces that light applies to the conduction electrons. Here, we describe the theory underlying the generation of drift currents in metals, particularly its application to photonic nanostructures using numerical simulations. We demonstrate that a gold photonic nanoantenna, optimized by a genetic algorithm, allows, under high excitation power, to maximize the drift currents and generate a pulse of stationary magnetic fields in the tesla range. This intense magnetic field, confined at the nanoscale and for a few femtoseconds, results from annular optical confinement and not from the creation of a single optical hot spot. Moreover, by controlling the incident polarization state, we demonstrate the orientation control of the created magnetic field and its reversal on demand. Finally, the stationary magnetic field's temporal behavior and the drift currents associated with it reveal the subcycle nature of this light-matter interaction. The manipulation of drift currents by a plasmonic nanostructure for the generation of stationary magnetic field pulses finds applications in the ultrafast control of magnetic domains with applications not only in data storage technologies but also in research fields such as magnetic trapping, magnetic skyrmion, magnetic circular dichroism, to spin control, spin precession, spin currents, and spin-waves, among others.

Nanophotonic approaches for nanoscale imaging and single-molecule detection at ultrahigh concentrations.

Over the last decade, we have witnessed an outburst of many different optical techniques aimed at breaking the diffraction limit of light, providing super-resolution imaging on intact fixed cells. In parallel, single-molecule detection by means of fluorescence has become a common tool to investigate biological interactions at the molecular level both in vitro and in living cells. Despite these advances, visualization of dynamic events at relevant physiological concentrations at the nanometer scale remains challenging. In this review, we focus on recent advancements in the field of nanophotonics toward nanoimaging and single-molecule detection at ultrahigh sample concentrations. These approaches rely on the use of metal nanostructures known as optical antennas to localize and manipulate optical fields at the nanometer scale. We highlight examples on how different optical antenna geometries are being implemented for nanoscale imaging of cell membrane components. We also discuss different implementations of self-standing and two-dimensional antenna arrays for studying nanoscale dynamics in living cell membranes as well as detection of individual biomolecular interactions in the µM range for sensing applications.

A plasmonic 'antenna-in-box' platform for enhanced single-molecule analysis at micromolar concentrations.

Single-molecule fluorescence techniques are key for a number of applications, including DNA sequencing, molecular and cell biology and early diagnosis. Unfortunately, observation of single molecules by diffraction-limited optics is restricted to detection volumes in the femtolitre range and requires pico- or nanomolar concentrations, far below the micromolar range where most biological reactions occur. This limitation can be overcome using plasmonic nanostructures, which enable the confinement of light down to nanoscale volumes. Although these nanoantennas enhance fluorescence brightness, large background signals and/or unspecific binding to the metallic surface have hampered the detection of individual fluorescent molecules in solution at high concentrations. Here we introduce a novel 'antenna-in-box' platform that is based on a gap-antenna inside a nanoaperture. This design combines fluorescent signal enhancement and background screening, offering high single-molecule sensitivity (fluorescence enhancement up to 1,100-fold and microsecond transit times) at micromolar sample concentrations and zeptolitre-range detection volumes. The antenna-in-box device can be optimized for single-molecule fluorescence studies at physiologically relevant concentrations, as we demonstrate using various biomolecules.