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The optical properties of phase-change materials (PCM) can be tuned to multiple levels by controlling the transition between their amorphous and crystalline phases. In multi-material PCM structures, the number of discrete reflectance levels can be increased according to the number of PCM layers. However, the effect of increasing number of layers on quenching and reversibility has not been thoroughly studied. In this work, the phase-change physics and thermal conditions required for reversible switching of single and multi-material PCM switches are discussed based on thermo-optical phase-change models and laser switching experiments. By using nanosecond laser pulses, 16 different reflectance levels in Ge2Sb2Te5 are demonstrated via amorphization. Furthermore, a multi-material switch based on Ge2Sb2Te5 and GeTe with four discrete reflectance levels is experimentally proven with a reversible multi-level response. The results and design principles presented herein will impact active photonics applications that rely on dynamic multi-level operation, such as optical computing, beam steering, and next-generation display technologies., Comment: 25 pages, 8 figures

Biological systems evolve with minimum metabolic costs and use common components, and they represent guideposts toward a paradigm of manufacturing that is centered on minimum energy, local resources, and ecological integration. Here, a new method of metalworking that uses chitosan from the arthropod cuticle to aggregate colloidal suspensions of different metals into solid ultra-low-binder-content composites is demonstrated. These composites, which can contain more than 99.5% metal, simultaneously show bonding affinity for biological components and metallic characteristics, such as electrical conductivity. This approach stands in contrast with existing metalworking methods, taking place at ambient temperature and pressure, and being driven by water exchange. Furthermore, all the nonmetallic components involved are metabolized in large amounts in every ecosystem. Under these conditions, the composites' ability to be printed and cast into functional shapes with metallic characteristics is demonstrated. The affinity of chitometallic composites for other biological components also allows them to infuse metallic characteristics into other biomaterials. The findings and robust manufacturing examples go well beyond basic demonstrations and offer a generalizable new approach to metalworking. The potential for a paradigm shift toward biomaterials based on their unique characteristics and the principles of their manufacturing methods is highlighted., Comment: 15 pages, 3 main figures, 4 videos, supplementary materials and methods, and 3 supplementary figures

Phase change memory devices are typically reset by melt-quenching a material to radically lower its electrical conductance. The high power and concomitantly high current density required to reset phase change materials is the major issue that limits the access times of 3D phase change memory architectures. Phase change superlattices were developed to lower the reset energy by confining the phase transition to the interface between two different phase change materials. However, the high thermal conductivity of the superlattices means that heat is poorly confined within the phase change material, and most of the thermal energy is wasted to the surrounding materials. Here, we identified Ti as a useful dopant for substantially lowering the thermal conductivity of Sb2Te3-GeTe superlattices whilst also stabilising the layered structure from unwanted disordering. We demonstrate via laser heating that lowering the thermal conductivity by doping the Sb2Te3 layers with Ti halves the switching energy compared to superlattices that only use interfacial phase change transitions and strain engineering. The thermally optimized superlattice has (0 0 l) crystallographic orientation yet a thermal conductivity of just 0.25 W/m.K in the "on" (set) state. Prototype phase change memory devices that incorporate this Ti-doped superlattice switch faster and and at a substantially lower voltage than the undoped superlattice. During switching the Ti-doped Sb2Te3 layers remain stable within the superlattice and only the Ge atoms are active and undergo interfacial phase transitions. In conclusion, we show the potential of thermally optimised Sb2Te3-GeTe superlattices for a new generation of energy-efficient electrical and optical phase change memory., Comment: 4 Figures, 7 Supplementary Figures, 27 pages including a supplement

All-dielectric metasurfaces provide unique solutions for advanced wavefront manipulation of light with complete control of amplitude and phase at sub-wavelength scales. One limitation, however, for most of these devices is the lack of any post-fabrication tunability of their response. To break this limit, a promising approach is employing phase-change-materials (PCM), which provide a fast, low energy and non-volatile means to endow metasurfaces with a switching mechanism. In this regard, great advancements have been done in the mid infrared and near infrared spectrum using different chalcogenides. In the visible spectral range, however, very few devices have demonstrated full phase manipulation, high efficiencies, and reversible switching. Here, we experimentally demonstrate a tunable all-dielectric Huygens metasurface made of antimony sulfide (Sb2S3) PCM, a low loss and high-index material in the visible spectral range with a large contrast (nearly 0.5) between its amorphous and crystalline states. We show close to 2pi phase modulation with high associated transmittance and use it to create switchable beam steering and holographic display devices. These novel chalcogenide PCM metasurfaces have the potential to emerge as a platform for next generation spatial light modulators and to impact application areas such as tunable and adaptive flat optics, LiDAR, and many more.

The switchable optical and electrical properties of phase change materials (PCMs) are finding new applications beyond data storage in reconfigurable photonic devices. However, high power heat pulses are needed to melt-quench the material from crystalline to amorphous. This is especially true in silicon photonics, where the high thermal conductivity of the waveguide material makes heating the PCM energy inefficient. Here, we improve the energy efficiency of the laser-induced phase transitions by inserting a layer of two-dimensional (2D) material, either MoS2 or WS2, between the silica or silicon and the PCM. The 2D material reduces the required laser power by at least 40% during the amorphization (RESET) process, depending on the substrate. Thermal simulations confirm that both MoS2 and WS2 2D layers act as a thermal barrier, which efficiently confines energy within the PCM layer. Remarkably, the thermal insulation effect of the 2D layer is equivalent to a ~100 nm layer of SiO2. The high thermal boundary resistance induced by the van der Waals (vdW)-bonded layers limits the thermal diffusion through the layer interfaces. Hence, 2D materials with stable vdW interfaces can be used to improve the thermal efficiency of PCM-tuned Si photonic devices. Furthermore, our waveguide simulations show that the 2D layer does not affect the propagating mode in the Si waveguide, thus this simple additional thin film produces a substantial energy efficiency improvement without degrading the optical performance of the waveguide. Our findings pave the way for energy-efficient laser-induced structural phase transitions in PCM-based reconfigurable photonic devices., Comment: 34 pages, 12 figures

Dielectric optical nanoantennas play an important role in color displays, metasurface holograms, and wavefront shaping applications. They usually exploit Mie resonances as supported on nanostructures with high refractive index, such as Si and TiO2. However, these resonances normally cannot be tuned. Although phase change materials, such as the germanium-antimony-tellurium alloys and post transition metal oxides, such as ITO, have been used to tune optical antennas in the near infrared spectrum, tunable dielectric antennae in the visible spectrum remain to be demonstrated. In this paper, we designed and experimentally demonstrated tunable dielectric nanoantenna arrays with Mie resonances in the visible spectrum, exploiting phase transitions in wide-bandgap Sb2S3 nano-resonators. In the amorphous state, Mie resonances in these Sb2S3 nanostructures give rise to a strong structural color in reflection mode. Thermal annealing induced crystallization and laser induced amorphization of the Sb2S3 resonators allow the color to be tuned reversibly. We believe these tunable Sb2S3 nanoantennae arrays will enable a wide variety of tunable nanophotonic applications, such as high-resolution color displays, holographic displays, and miniature LiDAR systems., Comment: 36 pages, 5 figures in main text, 9 figures in supporting information

Chalcogenide phase change materials (PCMs) have been extensively applied in data storage, and they are now being proposed for high resolution displays, holographic displays, reprogrammable photonics, and all-optical neural networks. These wide-ranging applications all exploit the radical property contrast between the PCMs different structural phases, extremely fast switching speed, long-term stability, and low energy consumption. Designing PCM photonic devices requires an accurate model to predict the response of the device during phase transitions. Here, we describe an approach that accurately predicts the microstructure and optical response of phase change materials during laser induced heating. The framework couples the Gillespie Cellular Automata approach for modelling phase transitions with effective medium theory and Fresnel equations. The accuracy of the approach is verified by comparing the PCM optical response and microstructure evolution with the results of nanosecond laser switching experiments. We anticipate that this approach to simulating the switching response of PCMs will become an important component for designing and simulating programmable photonics devices. The method is particularly important for predicting the multi-level optical response of PCMs, which is important for all-optical neural networks and PCM-programmable perceptrons., Comment: 26 pages, 6 figures

We designed and demonstrated a multi-spectral programmable perfect absorber that exploits two different phase-change materials. This programmability is possible by resonantly coupling two phase change materials, a Ge2Sb2Te5 layer to vanadium dioxide nanoparticles (VO2 NPs). The perfect absorption is attributed to the coalescence of gap plasmon modes excited between the NPs and waveguide cavity-like modes excited between the film and the NPs. The absorptance peak (>90%) can be tuned to four different infrared (IR) wavelengths from 1906 to 2960 nm by heating the structure to different temperatures. The perfect absorber is reconfigurable, lithography-free, large-scale, polarization-insensitive omnidirectional. Our strategy opens a new path for programmable infrared photonics.

Deeplearning algorithms are revolutionising many aspects of modern life. Typically, they are implemented in CMOS-based hardware with severely limited memory access times and inefficient data-routing. All-optical neural networks without any electro-optic conversions could alleviate these shortcomings. However, an all-optical nonlinear activation function, which is a vital building block for optical neural networks, needs to be developed efficiently on-chip. Here, we introduce and demonstrate both optical synapse weighting and all-optical nonlinear thresholding using two different effects in a chalcogenide material photonic platform. We show how the structural phase transitions in a wide-bandgap phase-change material enables storing the neural network weights via non-volatile photonic memory, whilst resonant bond destabilisation is used as a nonlinear activation threshold without changing the material. These two different transitions within chalcogenides enable programmable neural networks with near-zero static power consumption once trained, in addition to picosecond delays performing inference tasks not limited by wire charging that limit electrical circuits; for instance, we show that nanosecond-order weight programming and near-instantaneous weight updates enable accurate inference tasks within 20 picoseconds in a 3-layer all-optical neural network. Optical neural networks that bypass electro-optic conversion altogether hold promise for network-edge machine learning applications where decision-making in real-time are critical, such as for autonomous vehicles or navigation systems such as signal pre-processing of LIDAR systems.

High quality Van der Waals chalcogenides are important for phase change data storage, thermoelectrics, and spintronics. Using a combination of statistical design of experiments and density functional theory, we clarify how the out-of-equilibrium van der Waals epitaxial deposition methods can improve the crystal quality of Sb2Te3 films. We compare films grown by radio frequency sputtering and pulsed laser deposition (PLD). The growth factors that influence the crystal quality for each method are different. For PLD grown films a thin amorphous Sb2Te3 seed layer most significantly influences the crystal quality. In contrast, the crystalline quality of films grown by sputtering is rather sensitive to the deposition temperature and less affected by the presence of a seed layer. This difference is somewhat surprising as both methods are out-of-thermal-equilibrium plasma-based methods. Non-adiabatic quantum molecular dynamics simulations show that this difference originates from the density of excited atoms in the plasma. The PLD plasma is more intense and with higher energy than that used in sputtering, and this increases the electronic temperature of the deposited atoms, which concomitantly increases the adatom diffusion lengths in PLD. In contrast, the adatom diffusivity is dominated by the thermal temperature for sputter grown films. These results explain the wide range of Sb2Te3 and superlattice crystal qualities observed in the literature. These results indicate that, contrary to popular belief, plasma-based deposition methods are suitable for growing high quality crystalline chalcogenides., Comment: 24 pages, 8 figs

In the last decade phase change materials (PCM) research has switched from practical application in optical data storage toward electrical phase change random access memory technologies (PCRAM). As these devices are commercialised, we expect the research direction to switch once again toward electrical-photonic devices. The objective of this review is to introduce the concepts in PCM-tuned photonics. We will start by highlighting the key works in the field, before concentrating on PCM-tuned Metal-Dielectric-Metal (MDM) structures. We will discuss how to design tuneable-MDM photonics devices, their advantages, and their limitations. Finally we will discuss new materials for phase change photonics., Comment: 28 pages, 14 figures, adapted from a chapter to be published in the World Scientific Reference of Amorphous Materials

This work investigates the problematic diffusion of metal atoms into phase change chalcogenides, which can destroy resonances in photonic devices. Interfaces between Ge2Sb2Te5 and metal layers were studied using X-ray reflectivity (XRR) and reflectometry of metal-Ge2Sb2Te5 layered stacks. The diffusion of metal atoms influences the crystallisation temperature and optical properties of phase change materials. When Au, Ag, Al, W structures are directly deposited on Ge2Sb2Te5 inter-diffusion occurs. Indeed, Au forms AuTe2 layers at the interface. Diffusion barrier layers, such as Si3N4 or stable diffusionless plasmonic materials, such as TiN, can prevent the interfacial damage. This work shows that the interfacial diffusion must be considered when designing phase change material tuned photonic devices, and that TiN is the most suitable plasmonic material to interface directly with Ge2Sb2Te5., Comment: 23 pages, 8 figures, article

Light strongly interacts with structures that are of a similar scale to its wavelength; typically nanoscale features for light in the visible spectrum. However, the optical response of these nanostructures is usually fixed during the fabrication. Phase change materials offer a way to tune the properties of these structures in nanoseconds. Until now, phase change active photonics use materials that strongly absorb visible light, which limits their application in the visible spectrum. In contrast, Stibnite (Sb2S3) is an under-explored phase change material with a band gap that can be tuned in the visible spectrum from 2.0 to 1.7 eV. We deliberately couple this tuneable band gap to an optical resonator such that it responds dramatically in the visible spectrum to Sb2S3 reversible structural phase transitions. We show that this optical response can be triggered both optically and electrically. High speed reprogrammable Sb2S3 based photonic devices, such as those reported here, are likely to have wide applications in future intelligent photonic systems, holographic displays, and micro-spectrometers., Comment: 19 pages, 6 figures, submitted

Herein a genetic algorithm for optimising the design of layered 2D heterostructure is proposed. As a proof-of-concept it is applied to Sb$_2$Te$_3$-GeTe phase-change material superlattices, and the resulting lowest energy structure is grown experimentally. The similarity of the computational and experimental structures is verified with the comparison of XRD spectra. The structure is found to be within 0.92 meV/at. from the energetically most favorable known structure for Ge$_2$Sb$_2$Te$_5$.

Coherent phonons (CP) generated by laser pulses on the femtosecond scale have been proposed as a means to achieve ultrafast, non-thermal switching in phase-change materials such as Ge$_{2}$Sb$_{2}$Te$_{5}$(GST). Here we use ultrafast optical pump pulses to induce coherent acoustic phonons and stroboscopically measure the corresponding lattice distortions in GST using 100 ps x-ray pulses from the ESRF storage ring. A linear-chain model provides a good description of the observed changes in the diffraction signal, however, the magnitudes of the measured shifts are too large to be explained by thermal effects alone implying the presence of transient non-equilibrium electron heating in addition to temperature driven expansion. The information on the movement of atoms during the excitation process can lead to greater insight into the possibilities of using CP-induced phase-transitions in GST., Comment: 7 pages, 4 figures, Phys. Rev. B, in press