Control of Nanoscale Heat Generation with Lithography-Free Metasurface Absorbers.

Metasurfaces, artificially engineered surfaces comprised of subwavelength resonators, show promise for realizing a new generation of optical materials and devices. However, current metasurface architectures suffer from environmental degradation, a limited spectral range, and a lack of scalability. Here, we demonstrate a novel large-area embedded metasurface architecture that is environmentally robust and capable of a spectrally selective absorption of greater than 80% spanning from 330 to 2740 nm. These fully encapsulated metasurfaces leverage the capabilities of colloidal plasmonic nanoparticles with various crystallinities, materials, shapes, and sizes to access a larger spectral range and allow for control of nanoscale spatial losses and subsequent heat generation within the constituent elements of the metasurface. Through the selection of material, particle size, and shape, these metasurfaces can be designed across the ultraviolet (UV) to short-wave infrared (SWIR) region for various hot-electron, photodetection, photocatalysis, and photothermal processes.

Actively Tunable Metasurfaces via Plasmonic Nanogap Cavities with Sub-10-nm VO2 Films.

Actively tunable optical materials integrated with engineered subwavelength structures could enable novel optoelectronic devices, including reconfigurable light sources and tunable on-chip spectral filters. The phase-change material vanadium dioxide (VO2) provides a promising solid-state solution for dynamic tuning; however, previous demonstrations have been limited to thicker and often rough VO2 films or require a lattice-matched substrate for growth. Here, sub-10-nm-thick VO2 films are realized by atomic layer deposition (ALD) and integrated with plasmonic nanogap cavities to demonstrate tunable, spectrally selective absorption across 1200 nm in the near-infrared (NIR). Upon inducing the phase transition via heating, the absorption resonance is blue-shifted by as much as 60 nm. This process is reversible upon cooling and repeatable over more than ten temperature cycles. Dynamic, ultrathin VO2 films deposited by ALD, as demonstrated here, open up new potential architectures and applications where VO2 can be utilized to provide reconfigurability including three-dimensional, flexible and large-area structures.

Ultrafast pyroelectric photodetection with on-chip spectral filters.

Thermal detectors, such as bolometric, pyroelectric and thermoelectric devices, are uniquely capable of sensing incident radiation for any electromagnetic frequency; however, the response times of practical devices are typically on the millisecond scale1-7. By integrating a plasmonic metasurface with an aluminium nitride pyroelectric thin film, we demonstrate spectrally selective, room-temperature pyroelectric detectors from 660-2,000 nm with an instrument-limited 1.7 ns full width at half maximum and 700 ps rise time. Heat generated from light absorption diffuses through the subwavelength absorber into the pyroelectric film producing responsivities up to 0.18 V W-1 due to the temperature-dependent spontaneous polarization of the pyroelectric films. Moreover, finite-element simulations reveal the possibility of reaching a 25 ps full width at half maximum and 6 ps rise time rivalling that of semiconductor photodiodes8. This design approach has the potential to realize large-area, inexpensive gigahertz pyroelectric detectors for wavelength-specific detection from the ultraviolet to short-wave infrared or beyond for, for example, high-speed hyperspectral imaging.

Surpassing Single Line Width Active Tuning with Photochromic Molecules Coupled to Plasmonic Nanoantennas.

Active plasmonic nanostructures with tunable resonances promise to enable smart materials with multiple functionalities, on-chip spectral-based imaging and low-power optoelectronic devices. A variety of tunable materials have been integrated with plasmonic structures, however, the tuning range in the visible regime has been limited to less than the line width of the resonance resulting in small on/off ratios. Here we demonstrate dynamic tuning of plasmon resonances up to 71 nm through multiple cycles by incorporating photochromic molecules into plasmonic nanopatch antennas. Exposure to ultraviolet (UV) light switches the molecules into a photoactive state enabling dynamic control with on/off ratios up to 9.2 dB and a tuning figure of merit up to 1.43, defined as the ratio between the spectral shift and the initial line width of the plasmonic resonance. Moreover, the physical mechanisms underlying the large spectral shifts are elucidated by studying over 40 individual nanoantennas with fundamental resonances from 550 to 720 nm revealing good agreement with finite-element simulations.

Publisher Correction: Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface.

The originally published version of this Article contained an error in Equation 1. The two ℏ terms were missing from this equation. This has now been corrected in the PDF and HTML versions of the Article.

Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface.

The creation of energetic electrons through plasmon excitation of nanostructures before thermalization has been proposed for a wide number of applications in optical energy conversion and ultrafast nanophotonics. However, the use of "nonthermal" electrons is primarily limited by both a low generation efficiency and their ultrafast decay. We report experimental and theoretical results on the use of broadband plasmonic nanopatch metasurfaces comprising a gold substrate coupled to silver nanocubes that produce large concentrations of hot electrons, which we measure using transient absorption spectroscopy. We find evidence for three subpopulations of nonthermal carriers, which we propose arise from anisotropic electron-electron scattering within sp-bands near the Fermi surface. The bimetallic character of the metasurface strongly impacts the physics, with dissipation occurring primarily in the gold, whereas the quantum process of hot electron generation takes place in both components. Our calculations show that the choice of geometry and materials is crucial for producing strong ultrafast nonthermal electron components.The creation of energetic electrons through plasmon excitation has implications in optical energy conversion and ultrafast nanophotonics. Here, the authors find evidence for three subpopulations of nonthermal carriers which arise from anisotropic electron-electron scattering near the Fermi surface.

Toward Multispectral Imaging with Colloidal Metasurface Pixels.

Multispectral colloidal metasurfaces are fabricated that exhibit greater than 85% absorption and ≈100 nm linewidths by patterning film-coupled nanocubes in pixels using a fusion of bottom-up and top-down fabrication techniques over wafer-scale areas. With this technique, the authors realize a multispectral pixel array consisting of six resonances between 580 and 1125 nm and reconstruct an RGB image with 9261 color combinations.