Multi-mode lasing in supercell plasmonic nanoparticle arrays

Multicolour light sources can be used in applications such as lighting and multiplexing signals. In photonic and plasmonic systems, one way to achieve multicolour light is via multi-mode lasing. To achieve this, plasmonic nanoparticle arrays are typically arranged in superlattices that lead to multiple dispersions of the single arrays coupled via the superlattice Bragg modes. Here, we show an alternative way to enable multi-mode lasing in plasmonic nanoparticle arrays. We design a supercell in a square lattice by leaving part of the lattice sites empty. This results in multiple dispersive branches caused by the supercell period and hence creates additional band edges that can support lasing. We experimentally demonstrate multi-mode lasing in such a supercell array. Furthermore, we identify the lasing modes by calculating the dispersion by combining the structure factor of the array design with an empty lattice approximation. We conclude that the lasing modes are the 74th $\Gamma$- and 106th $X$-point of the supercell. By tuning the square lattice period with respect to the gain emission we can control the modes that lase. Finally, we show that the lasing modes exhibit a combination of transverse electric and transverse magnetic mode characteristics in polarization resolved measurements

Raman Enhancement in Bowtie-Shaped Aperture-Particle Hybrid Nanostructures Fabricated with DNA-Assisted Lithography

We report on efficient surface-enhanced Raman spectroscopy (SERS) supporting substrates, which are based on DNA-assisted lithography (DALI) and a layered configuration of materials. In detail, we used nanoscopic DNA origami bowtie templates to form hybrid nanostructures consisting of aligned silver bowtie-shaped particles and apertures of similar shape in a silver film. We hypothesized that this particular geometry could facilitate a four-fold advantage in Raman enhancement compared to common particle-based SERS substrates, and further, we verified these hypotheses experimentally and by finite difference time domain simulations. In summary, our DALI-fabricated hybrid structures suppress the background emission, allow emission predominantly from the areas of high field enhancement, and support additional resonances associated with the nanoscopic apertures. Finally, these nanoapertures also enhance the fields associated with the resonances of the underlying bowtie particles. The versatility and parallel nature of our DNA origami-based nanofabrication scheme and all of the above-mentioned features of the hybrid structures therefore make our optically resonant substrates attractive for various SERS-based applications.Comment: 7 pages, 4 figures, Supporting Information (5 pages, 3 tables, 1 figure

Thermal Control of Plasmonic Surface Lattice Resonances

Plasmonic metasurfaces exhibiting collective responses known as surface lattice resonances (SLRs) show potential for realizing tunable and flat photonic components for wavelength-selective processes, including lasing and optical nonlinearities. However, post-fabrication tuning of SLRs remains challenging, limiting the applicability of SLR-based components. Here, we demonstrate how the properties of high quality factor SLRs are easily modified by breaking the symmetry of the nanoparticle surroundings. We break the symmetry by changing the refractive index of the overlying immersion oil simply by controlling the ambient temperature of the device. We show that already modest temperature changes of 10{\deg}C can increase the quality factor of the investigated SLR from 400 to 750. Our results demonstrate accurate and reversible modification of the properties of the SLRs, paving the way towards tunable SLR-based photonic devices. On a more general level, our results demonstrate how symmetry breaking of the surrounding dielectric environment can be utilized for efficient and potentially ultrafast modification of the SLR properties

Phase-Matched Second-Harmonic Generation from Metasurfaces Inside Multipass Cells

We demonstrate a simple and scalable approach to increase conversion efficiencies of nonlinear metasurfaces by incorporating them into multipass cells and by letting the pump beam to interact with the metasurfaces multiple times. We experimentally show that by metasurface design, the associated phase-matching criteria can be fulfilled. As a proof of principle, we achieve phase matching of second-harmonic generation (SHG) using a metasurface consisting of aluminium nanoparticles deposited on a glass substrate. The phase-matching condition is verified to be achieved by measuring superlinear dependence of the detected SHG as a function of number of passes. We measure an order of magnitude enhancement in the SHG signal when the incident pump traverses the metasurface up to 9 passes. Results are found to agree well with a simple model developed to estimate the generated SHG signals. We also discuss strategies to further scale-up the nonlinear signal generation. Our approach provides a clear pathway to enhance nonlinear optical responses of metasurface-based devices. The generic nature of our approach holds promise for diverse applications in nonlinear optics and photonics

Nonlinear nonlocal metasurfaces

Optical metasurfaces have recently emerged as the game changer in light manipulation and opened up new perspectives in many subfields of optics and photonics. Recent developments in nonlocal metasurfaces, in which the nanoscale building blocks respond to the incoming light collectively rather than as individual objects, are especially promising for enhancing and controlling the nonlinear optical phenomena. In this article, we provide a brief overview of the basic principles of nonlocal metasurfaces in the context of their nonlinear optical functionalities. We discuss the origin and the regimes of the nonlocal response, covering the aspects of multiple scattering, radiation damping, quality factor, local-field enhancement, and temporal dynamics. Some important aspects are illustrated by computational examples. We also give our personal viewpoint on the selected ideas and research directions in nonlocal and nonlinear metasurfaces, including the role of spatial symmetry in nonlocal interactions, the effects of phase and momentum matching in frequency conversion, as well as the possibilities offered by new material platforms and novel concepts, such as bound states in the continuum, parity-time symmetry, and time-variant metasurfaces.publishedVersionPeer reviewe

Scattering dominated spatial coherence and phase correlation properties in plasmonic lattice lasers

We present a comprehensive study of the polarization and spatial coherence properties of the lasing modes supported by a four-fold symmetric plasmonic lattice. We can distinguish the scattering induced effects from the lattice geometry induced effects by modifying only the diameter of the particles while keeping the lattice geometry constant. Customized interferometric measurements reveal that the lasing emission undergoes a drastic change from 1D to 2D spatial coherence with increasing particle size, accompanied with dramatic changes in the far field polarization and beaming properties. By utilizing T-matrix scattering simulations, we reveal the physical mechanism governing this transition. In particular, we find that there exists increased radiative coupling in the diagonal directions at the plane of the lattice when the particle diameter is increased. Finally, we demonstrate that the x- and y-polarized (degenerate) lasing modes become phase locked with sufficiently large particles.publishedVersionPeer reviewe

Influence of enzyme immobilization and skin-sensor interface on non-invasive glucose determination from interstitial fluid obtained by magnetohydrodynamic extraction

We integrated a magnetohydrodynamic fluid extractor with an amperometric glucose biosensor to develop a wearable device for non-invasive glucose monitoring. Reproducible fluid extraction through the skin and efficient transport of the extracted fluid to the biosensor surface are prerequisites for non-invasive glucose monitoring. We optimized the enzyme immobilization and the interface layer between the sensing device and the skin. The monitoring device was evaluated by extracting fluid through porcine skin followed by glucose detection at the biosensor. The biosensor featured a screen-printed layer of Prussian Blue that was coated with a layer containing glucose oxidase. Both physical entrapment of glucose oxidase in chitosan and tethering of glucose oxidase to electrospun nanofibers were evaluated. Binding of glucose oxidase to nanofibers under mild conditions provided a stable biosensor with analytical performance suitable for accurate detection of micromolar concentrations of glucose. Hydrogels of varying thickness (95-2000 mu m) as well as a thin (30 mu m) nanofibrous polycaprolactone mat were studied as an interface layer between the biosensor and the skin. The effect of mass transfer phenomena at the biosensor-skin interface on the analytical performance of the biosensor was evaluated. The sensing device detected glucose extracted through porcine skin with an apparent (overall) sensitivity of-0.8 mA/(M.cm(2)), compared to a sensitivity of-17 mA/(M.cm(2)) for measurement in solution. The amperometric response of the biosensor correlated with the glucose concentration in the fluid that had been extracted through porcine skin with the magnetohydrodynamic technique.Peer reviewe

Strong coupling between surface plasmon polaritons and Sulforhodamine 101 dye

We demonstrate a strong coupling between surface plasmon polaritons and Sulforhodamine 101 dye molecules. Dispersion curves for surface plasmon polaritons on samples with a thin layer of silver covered with Sulforhodamine 101 molecules embedded in SU-8 polymer are obtained experimentally by reflectometry measurements and compared to the dispersion of samples without molecules. Clear Rabi splittings, with energies up to 360 and 190 meV, are observed at the positions of the dye absorption maxima. The split energies are dependent on the number of Sulforhodamine 101 molecules involved in the coupling process. Transfer matrix and coupled oscillator methods are used to model the studied multilayer structures with a great agreement with the experiments. Detection of the scattered radiation after the propagation provides another way to obtain the dispersion relation of the surface plasmon polaritons and, thus, provides insight into dynamics of the surface plasmon polariton/dye interaction, beyond the refrectometry measurements