Antenna-assisted picosecond control of nanoscale phase transition in vanadium dioxide

Nanoscale devices in which the interaction with light can be configured using external control signals hold great interest for next-generation optoelectronic circuits. Materials exhibiting a structural or electronic phase transition offer a large modulation contrast with multi-level optical switching and memory functionalities. In addition, plasmonic nanoantennas can provide an efficient enhancement mechanism for both the optically induced excitation and the readout of materials strategically positioned in their local environment. Here, we demonstrate picosecond all-optical switching of the local phase transition in plasmonic antenna-vanadium dioxide (VO2) hybrids, exploiting strong resonant field enhancement and selective optical pumping in plasmonic hotspots. Polarization- and wavelength-dependent pump-probe spectroscopy of multifrequency crossed antenna arrays shows that nanoscale optical switching in plasmonic hotspots does not affect neighboring antennas placed within 100 nm of the excited antennas. The antenna-assisted pumping mechanism is confirmed by numerical model calculations of the resonant, antenna-mediated local heating on a picosecond time scale. The hybrid, nanoscale excitation mechanism results in 20 times reduced switching energies and 5 times faster recovery times than a VO2 film without antennas, enabling fully reversible switching at over two million cycles per second and at local switching energies in the picojoule range. The hybrid solution of antennas and VO2 provides a conceptual framework to merge the field localization and phase-transition response, enabling precise, nanoscale optical memory functionalities

Phase-change-driven dielectric-plasmonic transitions in chalcogenide metasurfaces

Chalcogenides—alloys based on group-16 ‘chalcogen’ elements (sulfur, selenium, and tellurium) covalently bound to ‘network formers’ such as arsenic, germanium, antimony, and gallium—have a variety of technologically useful properties, including infrared transparency, high optical nonlinearity, photorefractivity and readily induced, reversible, non-volatile structural phase switching. Such phase-change materials are of enormous interest in the fields of plasmonics and nanophotonics. However, in such applications, the fact that some chalcogenides accrue plasmonic properties in the transition from an amorphous to a crystalline state, i.e., the real part of their relative permittivity becomes negative, has gone somewhat unnoticed. Indeed, one of the most commercially important chalcogenide compounds, germanium antimony telluride (Ge2:Sb2:Te5 or GST), which is widely used in rewritable optical and electronic data storage technologies, presents this behavior at wavelengths in the near-ultraviolet to visible spectral range. In this work, we show that the phase transition-induced emergence of plasmonic properties in the crystalline state can markedly change the optical properties of sub-wavelength-thickness, nanostructured GST films, allowing for the realization of non-volatile, reconfigurable (e.g., color-tunable) chalcogenide metasurfaces operating at visible frequencies and creating opportunities for developments in non-volatile optical memory, solid state displays and all-optical switching devices