We demonstrate reconfigurable phase-only computer-generated metasurface holograms with up to three image planes operating in the visible regime fabricated with gold nanorods on a stretchable polydimethylsiloxane substrate. Stretching the substrate enlarges the hologram image and changes the location of the image plane. Upon stretching, these devices can switch the displayed holographic image between multiple distinct images. This work opens up the possibilities for stretchable metasurface holograms as flat devices for dynamically reconfigurable optical communication and display. It also confirms that metasurfaces on stretchable substrates can serve as platform for a variety of reconfigurable optical devices.Keywords: flat optics; Metasurface; metasurface hologram; reconfigurable metasurface; tunable metasurface;

Active control of light-matter interactions in semiconductors is critical for realizing next generation optoelectronic devices with real-time control of the system’s optical properties and hence functionalities via external fields. The ability to dynamically manipulate optical interactions by applied fields in active materials coupled to cavities with fixed geometrical parameters opens up possibilities of controlling the lifetimes, oscillator strengths, effective mass, and relaxation properties of a coupled exciton–photon (or plasmon) system. Here, we demonstrate electrical control of exciton–plasmon coupling strengths between strong and weak coupling limits in a two-dimensional semiconductor integrated with plasmonic nanoresonators assembled in a field-effect transistor device by electrostatic doping. As a result, the energy-momentum dispersions of such an exciton–plasmon coupled system can be altered dynamically with applied electric field by modulating the excitonic properties of monolayer MoS2 arising from many-body effects. In addition, evidence of enhanced coupling between charged excitons (trions) and plasmons was also observed upon increased carrier injection, which can be utilized for fabricating Fermionic polaritonic and magnetoplasmonic devices. The ability to dynamically control the optical properties of a coupled exciton–plasmonic system with electric fields demonstrates the versatility of the coupled system and offers a new platform for the design of optoelectronic devices with precisely tailored responses.Keywords: 2D TMDC; electrical tuning; exciton plasmon polariton; magnetoplasmons; nanoplasmonics; trion plasmon;

Phase change materials (PCMs) are highly attractive for nonvolatile electrical and all-optical memory applications because of unique features such as ultrafast and reversible phase transitions, long-term endurance, and high scalability to nanoscale dimensions. Understanding their transient characteristics upon phase transition in both the electrical and the optical domains is essential for using PCMs in future multifunctional optoelectronic circuits. Here, we use a PCM nanowire embedded into a nanophotonic circuit to study switching dynamics in mixed-mode operation. Evanescent coupling between light traveling along waveguides and a phase-change nanowire enables reversible phase transition between amorphous and crystalline states. We perform time-resolved measurements of the transient change in both the optical transmission and resistance of the nanowire and show reversible switching operations in both the optical and the electrical domains. Our results pave the way toward on-chip multifunctional optoelectronic integrated devices, waveguide integrated memories, and hybrid processing applications.Keywords: All-optical switching; GeTe nanowires; nanophotonic circuits; phase change;

The field of plasmonics has attracted considerable attention in recent years because of potential applications in various fields such as nanophotonics, photovoltaics, energy conversion, catalysis, and therapeutics. It is becoming increasing clear that intrinsic high losses associated with plasmons can be utilized to create new device concepts to harvest the generated heat. It is therefore important to design cavities, which can harvest optical excitations efficiently to generate heat. We report a highly engineered nanowire cavity, which utilizes a high dielectric silicon core with a thin plasmonic film (Au) to create an effective metallic cavity to strongly confine light, which when coupled with localized surface plasmons in the nanoparticles of the thin metal film produces exceptionally high temperatures upon laser irradiation. Raman spectroscopy of the silicon core enables precise measurements of the cavity temperature, which can reach values as high as 1000 K. The same Si–Au cavity with enhanced plasmonic activity when coupled with TiO2 nanorods increases the hydrogen production rate by ∼40% compared to similar Au–TiO2 system without Si core, in ethanol photoreforming reactions. These highly engineered thermoplasmonic devices, which integrate three different cavity concepts (high refractive index core, metallo-dielectric cavity, and localized surface plasmons) along with the ease of fabrication demonstrate a possible pathway for designing optimized plasmonic devices with applications in energy conversion and catalysis.Keywords: cavity heating; Localized surface plasmons; metallo-dielectric cavity; nanowire; photoreforming; Raman spectroscopy; silicon; thermoplasmonics;

We demonstrate that optical second harmonic generation (SHG) can be utilized to determine the exact nature of nanotwins in noncentrosymmetric crystals, which is challenging to resolve via conventional transmission electron or scanned probe microscopies. Using single-crystalline nanotwinned CdTe nanobelts and nanowires as a model system, we show that SHG polarimetry can distinguish between upright (Cd–Te bonds) and inverted (Cd–Cd or Te–Te bonds) twin boundaries in the system. Inverted twin boundaries are generally not reported in nanowires due to the lack of techniques and complexity associated with the study of the nature of such defects. Precise characterization of the nature of defects in nanocrystals is required for deeper understanding of their growth and physical properties to enable their application in future devices.

Oxygen vacancy formation, migration, and subsequent agglomeration into conductive filaments in transition metal oxides under applied electric field is widely believed to be responsible for electroforming in resistive memory devices, although direct evidence of such a pathway is lacking. Here, by utilizing strong metal–support interaction (SMSI) between Pt and TiO2, we observe via transmission electron microscopy the electroforming event in lateral Pt/TiO2/Pt devices where the atomic Pt from the electrode itself acts as a tracer for the propagating oxygen vacancy front. SMSI, which originates from the d-orbital overlap between Pt atom and the reduced cation of the insulating oxide in the vicinity of oxygen vacancies, was optimized by fabricating nanoscale devices causing Pt atom migration tracking the moving oxygen vacancy front from the anode to cathode during electroforming. Experiments performed in different oxidizing and reducing conditions, which tune SMSI in the Pt-TiO2 system, further confirmed the role of oxygen vacancies during electroforming. These observations also demonstrate that the noble metal electrode may not be as inert as previously assumed.

We demonstrate strong exciton–plasmon coupling in silver nanodisk arrays integrated with monolayer MoS2 via angle-resolved reflectance microscopy spectra of the coupled system. Strong exciton–plasmon coupling is observed with the exciton–plasmon coupling strength up to 58 meV at 77 K, which also survives at room temperature. The strong coupling involves three types of resonances: MoS2 excitons, localized surface plasmon resonances (LSPRs) of individual silver nanodisks and plasmonic lattice resonances of the nanodisk array. We show that the exciton–plasmon coupling strength, polariton composition, and dispersion can be effectively engineered by tuning the geometry of the plasmonic lattice, which makes the system promising for realizing novel two-dimensional plasmonic polaritonic devices.

A mechanically reconfigurable metasurface that can continuously tune the wavefront is demonstrated in the visible frequency range by changing the lattice constant of a complex Au nanorod array fabricated on a stretchable polydimethylsiloxane substrate. It is shown that the anomalous refraction angle of visible light at 632.8 nm interacting with the tunable metasurface can be adjusted from 11.4° to 14.9° by stretching the substrate by ∼30%. An ultrathin flat 1.7× zoom lens whose focal length can continuously be changed from 150 to 250 μm is realized, which also demonstrates the potential of utilizing metasurfaces for reconfigurable flat optics.

We demonstrate the utility of optical second harmonic generation (SHG) polarimetry to perform structural characterization of noncentrosymmetric, single-crystalline II–VI semiconducting nanowires, nanobelts, and nanoflakes. By analyzing anisotropic SHG polarimetric patterns, we distinguish between wurtzite and zincblende II–VI semiconducting crystal structures and determine their growth orientation. The crystallography of these nanostructures was then confirmed via transmission electron microscopy measurements performed on the same system. In addition, we show that some intrinsic material properties such as nonlinear coefficients and geometry-dependent optical in-coupling coefficients can also be determined from the SHG experiments in WZ nanobelts. The ability to perform SHG-based structural characterization and crystallographic study of II–VI semiconducting single-crystalline nanomaterials will be useful to correlate structure–property relationships of nanodevices on which transmission electron microscopy measurements cannot be typically performed.

The manipulation of light-matter interactions in two-dimensional atomically thin crystals is critical for obtaining new optoelectronic functionalities in these strongly confined materials. Here, by integrating chemically grown monolayers of MoS2 with a silver-bowtie nanoantenna array supporting narrow surface-lattice plasmonic resonances, a unique two-dimensional optical system has been achieved. The enhanced exciton–plasmon coupling enables profound changes in the emission and excitation processes leading to spectrally tunable, large photoluminescence enhancement as well as surface-enhanced Raman scattering at room temperature. Furthermore, due to the decreased damping of MoS2 excitons interacting with the plasmonic resonances of the bowtie array at low temperatures stronger exciton–plasmon coupling is achieved resulting in a Fano line shape in the reflection spectrum. The Fano line shape, which is due to the interference between the pathways involving the excitation of the exciton and plasmon, can be tuned by altering the coupling strengths between the two systems via changing the design of the bowties lattice. The ability to manipulate the optical properties of two-dimensional systems with tunable plasmonic resonators offers a new platform for the design of novel optical devices with precisely tailored responses.

It has been observed that wurtzite II–VI semiconducting nanobelts transform into single-crystal, periodically branched nanostructures upon heating. The mechanism of this novel transformation has been elucidated by heating II–VI nanobelts in an environmental transmission electron microscope (ETEM) in oxidizing, reducing, and inert atmospheres while observing their structural changes with high spatial resolution. The interplay of surface reconstruction of high-energy surfaces of the wurtzite phase and environment-dependent anisotropic chemical etching of certain crystal surfaces in the branching mechanism of nanobelts has been observed. Understanding of structural and chemical transformations of materials via in situ microscopy techniques and their role in designing new nanostructured materials is discussed.

Structural defects and their dynamics play an important role in controlling the behavior of phase-change materials (PCM) used in low-power nonvolatile memory devices. However, not much is known about the influence of disorder on the electronic properties of crystalline PCM prior to a structural phase-change. Here, we show that the application of voltage pulses to single-crystalline GeTe nanowire memory devices introduces structural disorder in the form of dislocations and antiphase boundaries (APB). The dynamic evolution and pile-up of APBs increases disorder at a local region of the nanowire, which electronically transforms it from a metal to a dirty metal to an insulator, while still retaining single-crystalline long-range order. We also observe that close to this metal–insulator transition, precise control over the applied voltage is required to create an insulating state; otherwise the system ends up in a more disordered amorphous phase suggesting the role of electronic instabilities during the structural phase-change.

By integrating silicon nanowires (∼150 nm diameter, 20 μm length) with an Ω-shaped plasmonic nanocavity, we are able to generate broadband visible luminescence, which is induced by high order hybrid nanocavity-surface plasmon modes. The nature of this super bandgap emission is explored via photoluminescence spectroscopy studies performed with variable laser excitation energies (1.959 to 2.708 eV) and finite difference time domain simulations. Furthermore, temperature-dependent photoluminescence spectroscopy shows that the observed emission corresponds to radiative recombination of unthermalized (hot) carriers as opposed to a resonant Raman process.

Semiconductor nanostructures such as nanowires and nanoribbons functioning as Fabry–Pérot (F-P)-type optical cavities and nanolasers have attracted great interest not only for their potential use in nanophotonic systems but also to understand the physics of light–matter interactions at the nanoscale. Due to their nanoscale dimensions, new techniques need to be continuously developed to characterize the nature of highly confined optical modes. Furthermore, the inadequacy of typical far-field photoluminescence experiments for characterizing the nanoscale cavity modes such as parity and order has precluded efforts to obtain precise information that is required to fully understand these cavities. Here, we utilize a modified Young’s interference method based on angle-resolved microphotoluminescence spectral technique to directly reveal the parity of F-P cavity modes in CdS nanostructures functioning as waveguides and nanolasers. From these analyses, the mode order can be straightforwardly obtained with the help of numerical simulations. Moreover, we show that the Young’s technique is a general technique applicable to any F-P type cavities in nanoribbons, nanowires, or other photonic and plasmonic nanostructures.

Semiconductor nanowires, due to their unique electronic, optical, and chemical properties, are firmly placed at the forefront of nanotechnology research. The rich physics of semiconductor nanowire optics arises due to the enhanced light–matter interactions at the nanoscale and coupling of optical modes to electronic resonances. Furthermore, confinement of light can be taken to new extremes via coupling to the surface plasmon modes of metal nanostructures integrated with nanowires, leading to interesting physical phenomena. This Perspective will examine how the optical properties of semiconductor nanowires can be altered via their integration with highly confined plasmonic nanocavities that have resulted in properties such as orders of magnitude faster and more efficient light emission and lasing. The use of plasmonic nanocavities for tailored optical absorption will also be discussed in order to understand and engineer fundamental optical properties of these hybrid systems along with their potential for novel applications, which may not be possible with purely dielectric cavities.

Strain engineering can be utilized to tune the fundamental properties of semiconductor materials for applications in advanced electronic and photonic devices. Recently, the effects of large strain on the properties of nanostructures are being intensely investigated to further expand our insights into the physics and applications of such materials. In this Letter, we present results on controllable buckled cadmium-sulfide (CdS) optical nanowires (NWs), which show extremely large energy bandgap tuning by >250 meV with applied strains within the elastic deformation limit. Polarization and spatially resolved optical measurements reveal characteristics related to both compressive and tensile regimes, while microreflectance spectroscopy clearly demonstrates the effect of strain on the different types of excitons in CdS. Our results may enable strained NWs-based optoelectronic devices with tunable optical responses.

Increasing performance in organic/inorganic bulk heterojunctions hybrid photovoltaic systems hinges not only on the structure of the inorganic component but also on the morphology of the polymeric component. Changing the morphology of the organic component is a facile way of changing the morphology of the interface between the inorganic and organic components in the bulk heterojunction system. Engineering this interface to more efficiently split photogenerated excitons and transport these carriers to electrodes can increase the efficiency of photovoltaic devices. In this report, we investigate the effect of solvent quality on the morphology of the poly(3-hexylthiophene)-2,5-diyl (P3HT) polymer–semiconductor interface (solvatochromism). We have found that creating more order within the P3HT main chain in solution and prior to deposition has a profound effect on the nature of the P3HT-CdS nanowire interface. Solvents with a larger difference in solubility parameter, Δδ, relative to P3HT, such as methanol and isopropanol, create larger rod domains in the P3HT main chain and result in larger domains of crystalline P3HT at the interface. Solvents with similar solubility parameters as P3HT, such as pyridine and hexanol, create relatively shorter rod domains in the main chain and, as a result, nanohybrids with reduced crystallinity. The results of this paper further cement the importance of manipulating the rod–coil transition in the conducting polymers such as P3HT to improve the crystallinity at the polymer–semiconductor interface that can easily be scaled up to improve the efficiency of bulk heterojunction photovoltatic systems.

By combining high-resolution transmission electron microscopy (HRTEM) characterization and electrical measurements on a unique device platform, we study the reversible electrically-driven phase-change characteristics of self-assembled Ge2Sb2Te5 nanowires. Detailed HRTEM analyses are used to correlate and understand the effect of full and intermediate structural transformations on the measured electrical properties of the nanowire devices. The study demonstrates that our unique approach has the potential to provide new information regarding the dynamic structural and electrical states of phase-change materials at the nanoscale, which will aid the design of future phase-change memory devices.

Interfaces play an important role in bulk heterojunction organic/inorganic hybrid photovoltaic devices, but directly probing the interface in order to improve device characteristics is exceedingly difficult. We report on a method to form core–shell inorganic nanowire–polymer hybrids of a conducting polymer, poly(3-hexlthiophene-2,5-diyl) (P3HT), and a semiconducting nanowire, cadmium sulfide (CdS), using solution processing to create the polymer shell around the nanowire in order to study the polymer–nanowire interface directly without interference from bulk effects. We have used the rod–coil transition (chromism) in P3HT to seed and enhance the crystallinity at the polymer–nanowire interface. We have shown that creating more order within the P3HT main chain, by controlling the temperature and the solvent quality, can increase the extent of polymer crystallinity present at the polymer–nanowire interface. We believe using the rod–coil transition to create more order in P3HT and the resulting polymer–nanowire interface will provide a facile pathway for designing future organic–inorganic photovoltaic devices.

Semiconductor nanowire waveguide cavities hold promise for nanophotonic applications such as lasers, waveguides, switches, and sensors due to the tight optical confinement in these structures. However, to realize their full potential, high quality nanowires, whose emission at low temperatures is dominated by free exciton emission, need to be synthesized. In addition, a proper understanding of their complex optical properties, including light-matter coupling in these subwavelength structures, is required. We have synthesized very high-quality wurztite CdS nanowires capped with a 5 nm SiO2 conformal coating with diameters spanning 100−300 nm using physical vapor and atomic layer deposition techniques and characterized their spatially resolved photoluminescence over the 77−298 K temperature range. In addition to the Fabry−Pérot resonator modulated emission from the ends of the wires, the low temperature emission from the center of the wire shows clear free excitonic peaks and LO phonon replicas, persisting up to room-temperature in the passivated wires. From laser scanning measurements we determined the absorption in the vicinity of the excitonic resonances. In addition to demonstrating the high optical quality of the nanowire crystals, these results provide the fundamental parameters for strong light-matter coupling studies, potentially leading to low threshold polariton lasers, sensitive sensors and optical switches at the nanoscale.

The unique properties of nanostructured materials enable their transformation into complex, kinetically controlled morphologies that cannot be obtained during their growth. Solution-phase cation-exchange reactions can transform sub-10 nm nanocrystals/nanorods into varying compositions and superlattice structures; however, because of their small size, cation-exchange reaction rates are extremely fast, which limits control over the transformed products and possibilities for obtaining new morphologies. Nanowires are routinely synthesized via gas-phase reactions with 5−200 nm diameters, and their large aspect ratios allow them to be electrically addressed individually. To realize their full potential, it is desirable to develop techniques that can transform nanowires into tunable but precisely controlled morphologies, especially in the gas-phase, to be compatible with nanowire growth schemes. We report transformation of single-crystalline cadmium sulfide nanowires into composition-controlled ZnxCd(1−x)S nanowires, core−shell heterostructures, metal-semiconductor superlattices (Zn−ZnxCd(1−x)S), single-crystalline ZnS nanotubes, and eventually metallic Zn nanowires by utilizing size-dependent cation-exchange reaction along with temperature and gas-phase reactant delivery control. This versatile synthetic ability to transform nanowires offers new opportunities to study size-dependent phenomena at the nanoscale and tune their chemical/physical properties to design reconfigurable circuits.

A new technique is reported where by combining spatially and spectrally resolved scanning optical microscopy on single nanowire active waveguides, waveguide propagation loss and dispersion can be determined. The waveguide propagation loss spectra have been utilized to obtain insights into the optical absorption spectra of these unique nanostructured materials, which are modified in comparison to bulk materials. The propagation spectra and waveguide dispersion show clear signatures of electronic effects such as exciton−polariton formation. These results show the importance of the polaritonic nature of waveguiding in semiconducting nanoscale optical cavities and provide insights for the integration of semiconductor nanowire waveguides in nanophotonic circuitry.

Fundamental understanding of the size dependence of nanoscale optical confinement in semiconductor nanowire waveguides, as expressed by changes in the dispersion of light, is crucial for the optimal design of nanophotonic devices. Measurements of the dispersion are particularly challenging for nanoscale cavities due to difficulties associated with the in- and out-coupling of light resulting from diffraction effects. We report the strong size dependence of optical dispersion and associated group velocities in subwavelength width ZnSe nanowire waveguide cavities, using a technique based on Fabry-Pérot resonator modes as probes over a wide energy range. Furthermore, we observed subwavelength (λ/9) dispersionless waveguiding and significant slowing of the propagating light by 90% (c/8). These results, in addition to providing insights into nanoscale optical transport, will facilitate the rational design of nanowire photonic devices with tailored dispersion and group velocities.

We report the synthesis and characterization of phase-change Ge−Sb nanowires with two different eutectic compositions and their memory switching characteristics. Under application of electric-fields with controlled pulse amplitude and duration times, Sb-rich (Sb ≥ 86 at. %) eutectic Ge−Sb nanowires show phase-change based memory switching, while another eutectic GeSb (Ge:Sb = 1:1) nanowires do not show electronic memory switching at all. However, under repeated measurements, Sb-rich Ge−Sb nanowires display an increase of resistance of the low resistive state. The observed electrical irreversibility for Sb-rich Ge−Sb nanowires is attributed to the structural and compositional instability due to the phase-separation of Ge out of homogeneous Ge−Sb as observed from rapid thermal annealing and transmission electron microscopy experiments. Implications for design of Te-free nanoscale materials for phase change memory applications are also discussed.

We report self-assembly of highly aligned GeTe nanowires epitaxially grown on octahedral GeTe microcrystals in two well-defined directions by using one-step vapor transport process. The epitaxial relationship of nanowires with underlying microcrystals along with the growth orientations of nanowires were investigated in detail by electron microscopy combined with atomic unit cell models. We demonstrate that maximizing atomic planar density to minimize energy of the exposed surfaces is the determining factor that governs the unique growth characteristics of micro/nanostructures that evolve from three-dimensional octahedral microcrystals to tetrahedral bases to finally one-dimensional nanowires. The crystallographic understanding of structuring of crystalline nanomaterials obtained from this study will be critical to understand, predict, and control the growth orientation of nanostructures in three-dimensions.

The ability to control the size of nanostructures still presents one of the biggest challenges in nanosciences. While impressive progress has been made toward diameter-controlled synthesis of nanocrystals via solution-phase chemical techniques, control over nanowire diameters grown via the gas-phase vapor−liquid−solid mechanism is still challenging. Diameter-controlled growth of nanowires have been reported by controlling the size of the metal nanocatalysts, which is a general technique. However, the complex dynamics of gas-phase reactants and their reaction with catalysts requires in-depth understanding of the effect of various growth parameters on the size of catalysts during growth, which makes diameter-controlled growth of nanowires challenging. Here, we report diameter-controlled growth of GeTe nanowires, which are important materials for phase-change memory devices. Recently, several groups have investigated phase-change nanowires for memory applications, but the ability to control their diameters has been lacking. This lack of nanowire size control has made investigation of phase-change memory switching difficult for both fundamental science and device applications. We find that by controlling the rate of supercooling and the reactant supply rate we can produce large quantities of nanowires with uniform, narrow diameter distributions. The effects of various growth parameters such as temperature, pressure, and reactant supply rate on nanowire morphologies are discussed.

Phase-change memory, which switches reversibly between crystalline and amorphous phases, is promising for next generation data-storage devices. In this work, we present a novel, nonbinary data-storage device using core−shell nanowires to significantly enhance memory capacity by combining two phase-change materials with different electronic and thermal properties to engineer different onsets of amorphous-crystalline transitions. Electric-field induced sequential amorphous-crystalline transition in core−shell nanowires displays three distinct electronic states with high, low, and intermediate resistances, assigned as data “0”, “1”, and “2”.

By combining electron microscopy and size-dependent electrical measurements, we demonstrate surface-induced heterogeneous nucleation-dominant mechanism for recrystallization of amorphous phase-change Ge2Sb2Te5 nanowires. Heterogeneous nucleation theory quantitatively predicts the nucleation rates that vary by 5 orders of magnitude from 190 to 20 nm lengthscales. Our work demonstrates that increasing the surface-to-volume ratio of nanowires has two effects: lowering of the activation energy barrier due to phonon instability and providing nucleation sites for recrystallization. The systematic study of the effect of surface in phase-change behavior is critical for understanding nanoscale phase-transitions and design of nonvolatile memory devices.

We demonstrate a general approach for growing vertically aligned, single-crystalline nanowires of any material on arbitrary substrates by using plasma-sputtered Au/Pd thin films as a catalyst through the vapor−liquid−solid process. The high-energy sputtered Au/Pd atoms form a reactive interface with the substrate forming nanoclusters which get embedded in the substrate, thus providing mechanical stability for vertically aligned nanowire growth. We demonstrate that our approach for vertically aligned nanowire growth is generic and can be extended to various complex substrates such as conducting indium tin oxide.