Lanthanide-doped upconversion nanocrystals (UCNCs) have recently become an attractive nonlinear fluorescence material for use in bioimaging because of their tunable spectral characteristics and exceptional photostability. Plasmonic materials are often introduced into the vicinity of UCNCs to increase their emission intensity by means of enlarging the absorption cross-section and accelerating the radiative decay rate. Moreover, plasmonic nanostructures (e.g., gold nanorods, GNRs) can also influence the polarization state of the UC fluorescence—an effect that is of fundamental importance for fluorescence polarization-based imaging methods yet has not been discussed previously. To study this effect, we synthesized GNR@SiO2@CaF2:Yb3+,Er3+ hybrid core–shell–satellite nanostructures with precise control over the thickness of the SiO2 shell. We evaluated the shell thickness-dependent plasmonic enhancement of the emission intensity in ensemble and studied the plasmonic modulation of the emission polarization at the single-particle level. The hybrid plasmonic UC nanostructures with an optimal shell thickness exhibit an improved bioimaging performance compared with bare UCNCs, and we observed a polarized nature of the light at both UC emission bands, which stems from the relationship between the excitation polarization and GNR orientation. We used electrodynamic simulations combined with Förster resonance energy transfer theory to fully explain the observed effect. Our results provide extensive insights into how the coherent interaction between the emission dipoles of UCNCs and the plasmonic dipoles of the GNR determines the emission polarization state in various situations and thus open the way to the accurate control of the UC emission anisotropy for a wide range of bioimaging and biosensing applications.

Nanoscale devices -such as all-optical modulators and electro-optical transducers -can be implemented in heterostructures that integrate plasmonic nanostructures with functional active materials.Here we demonstrate all-optical control of a nanoscale memory effect in such a heterostructure by coupling the localized surface plasmon resonance (LSPR) of gold nanodisk arrays to a phase-changing material (PCM), vanadium dioxide (VO 2 ). By latching the VO 2 in a distinct correlated metallic state during the insulator-to-metal transition (IMT), while concurrently exciting the hybrid nanostructure with one or more ultraviolet optical pulses, the entire phase space of this correlated state can be accessed optically to modulate the plasmon response. We find that the LSPR modulation depends strongly but linearly on the initial latched state, suggesting that the memory effect encoded in the plasmon resonance wavelength is linked to the strongly correlated electron states of the VO 2 . The continuous, linear variation of the electronic and optical properties of these model heterostructures opens the way to multiple design strategies for hybrid devices with novel optoelectronic functionalities, which can be controlled by an applied electric or optical field, strain, injected charge or temperature.

Metasurfaces offer unparalleled functionalities for controlling the propagation and properties of electromagnetic waves. But to transfer these functions to technological applications, it is critical to render them tunable and to enable fast control by external stimuli. In most cases, this has been realized by utilizing tunable materials combined with a top-down nanostructuring process, which is often complicated and time intensive. Here we present a novel strategy for fabricating a tunable metasurface comprising epitaxially grown nanobeams of a phase transition material, vanadium dioxide. Without the need for extensive nanolithographic fabrication, we prepared a large-area (>1 cm 2 ), deep-subwavelength (thickness of ∼λ/40) nanostructured thin film that can control light transmission with large modulation depth, exceeding 9 dB across all telecommunication wavelength bands. Furthermore, the transmission in the "on" state remains higher than 80% from near-to mid-infrared region. This renders our metasurface useful also as a phase-shifting element, which we demonstrate by carrying out cross-polarized transmission measurements. To provide insights about the relationship between metasurface morphology and its resulting optical properties, we perform full-field three-dimensional numerical simulations as a function of width, height, and edge-to-edge separation of the epitaxial VO 2 nanobeams.

Colloidal gold nanoparticles represent technological building blocks which are easy to fabricate while keeping full control of their shape and dimensions. Here, we report on a simple two-step maskless process to assemble gold nanoparticles from a water colloidal solution at specific sites of a silicon surface. First, the silicon substrate covered by native oxide is exposed to a charged particle beam (ions or electrons) and then immersed in a HF-modified solution of colloidal nanoparticles. The irradiation of the native oxide layer by a low-fluence charged particle beam causes changes in the type of surface-terminating groups, while the large fluences induce even more profound modification of surface composition. Hence, by a proper selection of the initial substrate termination, solution pH, and beam fluence, either positive or negative deposition of the colloidal nanoparticles can be achieved.

We present an experimental and theoretical study of Babinet’s principle of complementarity in plasmonics. We have used spatially-resolved electron energy loss spectroscopy and cathodoluminescence to investigate electromagnetic response of elementary plasmonic antenna: gold discs and complementary disc-shaped apertures in a gold layer. We have also calculated their response to the plane wave illumination. While the qualitative validity of Babinet’s principle has been confirmed, quantitative differences have been found related to the energy and quality factor of the resonances and the magnitude of related near fields. In particular, apertures were found to exhibit stronger interaction with the electron beam than solid antennas, which makes them a remarkable alternative of the usual plasmonic-antennas design. We also examine the possibility of magnetic near field imaging based on the Babinet’s principle.

Metasurfaces are ultrathin nanostructured surfaces that can allow arbitrary manipulation of light. Implementing dynamic tunability into their design could allow the optical functions of metasurfaces to be rapidly modified at will. The most pronounced and robust tunability of optical properties is provided by phase-change materials such as vanadium dioxide (VO2) and germanium antimony telluride (GST), but their implementations have been limited only to near-infrared wavelengths. Here, we demonstrate that VO2 nanoantennas with widely tunable Mie resonances can be utilized for designing tunable metasurfaces in the visible range. In contrast to the dielectric-metallic phase transition-induced tunability in previous demonstrations, we show that dielectric Mie resonances in VO2 nanoantennas offer remarkable scattering and extinction modulation depths (5−8 dB and 1−3 dB, respectively) for tunability in the visible. Moreover, these strong resonances are optically switchable using a continuous-wave laser. Our results establish VO2 nanostructures as low-loss building blocks of optically tunable metasurfaces.

Optical metasurfaces have emerged as a new generation of building blocks for multi-functional optics. Design and realization of metasurface elements place ever-increasing demands on accurate assessment of phase alterations introduced by complex nanoantenna arrays, a process referred to as quantitative phase imaging. Despite considerable effort, the widefield (non-scanning) phase imaging that would approach resolution limits of optical microscopy and indicate the response of a single nanoantenna still remains a challenge. Here, we report on a new strategy in incoherent holographic imaging of metasurfaces, in which unprecedented spatial resolution and light sensitivity are achieved by taking full advantage of the polarization selective control of light through the geometric (Pancharatnam-Berry) phase. The measurement is carried out in an inherently stable common-path setup composed of a standard optical microscope and an add-on imaging module. Phase information is acquired from the mutual coherence function attainable in records created in broadband spatially incoherent light by the self-interference of scattered and leakage light coming from the metasurface. In calibration measurements, the phase was mapped with the precision and spatial background noise better than 0.01 rad and 0.05 rad, respectively. The imaging excels at the high spatial resolution that was demonstrated experimentally by the precise amplitude and phase restoration of vortex metalenses and a metasurface grating with 833 lines/mm. Thanks to superior light sensitivity of the method, we demonstrated, for the first time to our knowledge, the widefield measurement of the phase altered by a single nanoantenna, while maintaining the precision well below 0.15 rad.

Coherence-controlled holographic microscopy (CCHM) is a realtime, wide-field, and quantitative light-microscopy technique enabling 3D imaging of electromagnetic fields, providing complete information about both their intensity and phase. These attributes make CCHM a promising candidate for performance assessment of phase-altering metasurfaces, a new class of artificial materials that allow to manipulate the wavefront of passing light and thus provide unprecedented functionalities in optics and nanophotonics. In this paper, we report on our investigation of phase imaging of plasmonic metasurfaces using holographic microscopy. We demonstrate its ability to obtain phase information from the whole field of view in a single measurement on a prototypical sample consisting of silver nanodisc arrays. The experimental data were validated using FDTD simulations and a theoretical model that relates the obtained phase image to the optical response of metasurface building blocks. Finally, in order to reveal the full potential of CCHM, we employed it in the analysis of a simple metasurface represented by a plasmonic zone plate. By scanning the sample along the optical axis we were able to create a quantitative 3D phase map of fields transmitted through the zone plate. The presented results prove that CCHM is inherently suited to the task of metasurface characterization. Moreover, as the temporal resolution is limited only by the camera framerate, it can be even applied in analysis of actively tunable metasurfaces.