Localized Nanoresonator Mode in Plasmonic Microcavities.

Submicron-thick hexagonal boron nitride crystals embedded in noble metals form planar Fabry-Perot half-microcavities. Depositing Au nanoparticles on top of these microcavities forms previously unidentified angle- and polarization-sensitive nanoresonator modes that are tightly laterally confined by the nanoparticle. Comparing dark-field scattering with reflection spectroscopies shows plasmonic and Fabry-Perot-like enhancements magnify subtle interference contributions, which lead to unexpected redshifts in the dark-field spectra, explained by the presence of these new modes.

Electrical Tuning of Nonlinearities in Exciton-Polariton Condensates.

A primary limitation of the intensively researched polaritonic systems compared to their atomic counterparts for the study of strongly correlated phenomena and many-body physics is their relatively weak two-particle interactions compared to disorder. Here, we show how new opportunities to enhance such on-site interactions and nonlinearities arise by tuning the exciton-polariton dipole moment in electrically biased semiconductor microcavities incorporating wide quantum wells. The applied field results in a twofold enhancement of exciton-exciton interactions as well as more efficiently driving relaxation towards low energy polariton states, thus, reducing condensation threshold.

Spin Order and Phase Transitions in Chains of Polariton Condensates.

We demonstrate that multiply coupled spinor polariton condensates can be optically tuned through a sequence of spin-ordered phases by changing the coupling strength between nearest neighbors. For closed four-condensate chains these phases span from ferromagnetic (FM) to antiferromagnetic (AFM), separated by an unexpected crossover phase. This crossover phase is composed of alternating FM-AFM bonds. For larger eight-condensate chains, we show the critical role of spatial inhomogeneities and demonstrate a scheme to overcome them and prepare any desired spin state. Our observations thus demonstrate a fully controllable nonequilibrium spin lattice.

Plasmonic response and SERS modulation in electrochemical applied potentials.

We study the optical response of individual nm-wide plasmonic nanocavities using a nanoparticle-on-mirror design utilised as an electrode in an electrochemical cell. In this geometry Au nanoparticles are separated from a bulk Au film by an ultrathin molecular spacer, giving intense and stable Raman amplification of 100 molecules. Modulation of the plasmonic spectra and the SERS response is observed with an applied voltage under a variety of electrolytes. Different scenarios are discussed to untangle the various mechanisms that can be involved in the electronic interaction between NPs and electrode surfaces.

Tracking Nanoelectrochemistry Using Individual Plasmonic Nanocavities.

We study in real time the optical response of individual plasmonic nanoparticles on a mirror, utilized as electrodes in an electrochemical cell when a voltage is applied. In this geometry, Au nanoparticles are separated from a bulk Au film by an ultrathin molecular spacer. The nanoscale plasmonic hotspot underneath the nanoparticles locally reveals the modified charge on the Au surface and changes in the polarizability of the molecular spacer. Dark-field and Raman spectroscopy performed on the same nanoparticle show our ability to exploit isolated plasmonic junctions to track the dynamics of nanoelectrochemistry. Enhancements in Raman emission and blue-shifts at a negative potential show the ability to shift electrons within the gap molecules.

Tracking Optical and Electronic Behaviour of Quantum Contacts in Sub-Nanometre Plasmonic Cavities.

Plasmonic interactions between two metallic tips are dynamically studied in a supercontinuum dark-field microscope and the transition between coupled and charge-transfer plasmons is directly observed in the sub-nm regime. Simultaneous measurement of the dc current, applied force, and optical scattering as the tips come together is used to determine the effects of conductive pathways within the plasmonic nano-gap. Critical conductances are experimentally identified for the first time, determining the points at which quantum tunnelling and conductive charge transport begin to influence plasmon coupling. These results advance our understanding of the relationship between conduction and plasmonics, and the fundamental quantum mechanical behaviours of plasmonic coupling.

Tracking Optical Welding through Groove Modes in Plasmonic Nanocavities.

We report the light-induced formation of conductive links across nanometer-wide insulating gaps. These are realized by incorporating spacers of molecules or 2D monolayers inside a gold plasmonic nanoparticle-on-mirror (NPoM) geometry. Laser irradiation of individual NPoMs controllably reshapes and tunes the plasmonic system, in some cases forming conductive bridges between particle and substrate, which shorts the nanometer-wide plasmonic gaps geometrically and electronically. Dark-field spectroscopy monitors the bridge formation in situ, revealing strong plasmonic mode mixing dominated by clear anticrossings. Finite difference time domain simulations confirm this spectral evolution, which gives insights into the metal filament formation. A simple analytic cavity model describes the observed plasmonic mode hybridization between tightly confined plasmonic cavity modes and a radiative antenna mode sustained in the NPoM. Our results show how optics can reveal the properties of electrical transport across well-defined metallic nanogaps to study and develop technologies such as resistive memory devices (memristors).

Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates.

Tunable spin correlations are found to arise between two neighboring trapped exciton-polariton condensates which spin polarize spontaneously. We observe a crossover from an antiferromagnetic to a ferromagnetic pair state by reducing the coupling barrier in real time using control of the imprinted pattern of pump light. Fast optical switching of both condensates is then achieved by resonantly but weakly triggering only a single condensate. These effects can be explained as the competition between spin bifurcations and spin-preserving Josephson coupling between the two condensates, and open the way to polariton Bose-Hubbard ladders.

Controlling Nanowire Growth by Light.

Individual Au catalyst nanoparticles are used for selective laser-induced chemical vapor deposition of single germanium nanowires. Dark-field scattering reveals in real time the optical signatures of all key constituent growth processes. Growth is initially triggered by plasmonic absorption in the Au catalyst, while once nucleated the growing Ge nanowire supports magnetic and electric resonances that then dominate the laser interactions. This spectroscopic understanding allows real-time laser feedback that is crucial toward realizing the full potential of controlling nanomaterial growth by light.

Nonlinear superchiral meta-surfaces: tuning chirality and disentangling non-reciprocity at the nanoscale.

Circularly polarized light is incident on a nanostructured chiral meta-surface. In the nanostructured unit cells whose chirality matches that of light, superchiral light is forming and strong optical second harmonic generation can be observed.

Optical superfluid phase transitions and trapping of polariton condensates.

Semiconductor microcavities are used to support freely flowing polariton quantum liquids allowing the direct observation and optical manipulation of macroscopic quantum states. Incoherent optical excitation at a point produces radially expanding condensate clouds within the planar geometry. By using arbitrary configurations of multiple pump spots, we discover a geometrically controlled phase transition, switching from the coherent phase-locking of multiple condensates to the formation of a single trapped condensate. The condensation threshold becomes strongly dependent on the programmed superfluid geometry and sensitive to cooperative interactions between condensates. We directly image persistently circulating superfluid and show how flows of light-matter quasiparticles are dominated by the quantum pressure in such configurable laser-written potential landscapes.

Self-sifting of chain plasmons: the complex optics of Au nanoparticle clusters.

The strong enhancement of electrical fields in subnanometer gaps of self-assembled gold nanoparticle clusters holds great promise for large scale fabrication of sensitive optical sensing substrates. Due to the large number of involved nanoparticles, however, their optical response is complex and not easily accessible through numerical simulations. Here, we use hyperspectral supercontinuum spectroscopy to demonstrate how confined optical modes of well defined energies are supported by different areas of the cluster. Due to the strong resonant coupling in those regions, the cluster essentially acts as a nanoscale optical sieve which sorts incident light according to its wavelength.

Geometrically locked vortex lattices in semiconductor quantum fluids.

Macroscopic quantum states can be easily created and manipulated within semiconductor microcavity chips using exciton-photon quasiparticles called polaritons. Besides being a new platform for technology, polaritons have proven to be ideal systems to study out-of-equilibrium condensates. Here we harness the photonic component of such a semiconductor quantum fluid to measure its coherent wavefunction on macroscopic scales. Polaritons originating from separated and independent incoherently pumped spots are shown to phase-lock only in high-quality microcavities, producing up to 100 vortices and antivortices that extend over tens of microns across the sample and remain locked for many minutes. The resultant regular vortex lattices are highly sensitive to the optically imposed geometry, with modulational instabilities present only in square and not triangular lattices. Such systems describe the optical equivalents to one- and two-dimensional spin systems with (anti)-ferromagnetic interactions controlled by their symmetry, which can be reconfigured on the fly, paving the way to widespread applications in the control of quantum fluidic circuits.

Corrugated metallodielectric superlattices via release-rollup assembly.

A 'release-rollup' assembly (RRA) technique is described that yields corrugated metallodielectric superlattices. Bilayers of polymer/Au cast onto diffraction gratings are released and rolled into multilayers with registration of the stacked corrugations across mm-scales. Optical imaging reveals Moiré fringes with reflection spectra that track the bilayer thickness due to mis-stacking. Angular-resolved spectra show spectrally-modulated diffraction opposite to that of the metallic stop-bands, but which agrees with a simple model. This scalable fabrication strategy is thus widely exploitable for laterally patterned metamaterials and optical superlattices.

Enhancing solar cells with localized plasmons in nanovoids.

Localized plasmon resonances of spherical nanovoid arrays strongly enhance solar cell performance by a factor of 3.5 in external quantum efficiency at plasmonic resonances, and a four-fold enhancement in overall power conversion efficiency. Large area substrates of silver nanovoids are electrochemically templated through self-assembled colloidal spheres and organic solar cells fabricated on top. Our design represents a new class of plasmonic photovoltaic enhancement: that of localized plasmon-enhanced absorption within nanovoid structures. Angularly-resolved spectra demonstrate strong localized Mie plasmon modes within the nanovoids. Theoretical modelling shows varied spatial dependence of light intensity within the void region suggesting a first possible route towards Third Generation plasmonic photovoltaics.

Bragg polaritons: strong coupling and amplification in an unfolded microcavity.

Periodic incorporation of quantum wells inside a one-dimensional Bragg structure is shown to enhance coherent coupling of excitons to the electromagnetic Bloch waves. We demonstrate strong coupling of quantum well excitons to photonic crystal Bragg modes at the edge of the photonic band gap, which gives rise to mixed Bragg polariton eigenstates. The resulting Bragg polariton branches are in good agreement with the theory and allow demonstration of Bragg polariton parametric amplification.

Shear ordering in polymer photonic crystals.

Optical scattering spectra are recorded in situ on flowing colloidal polymeric nanocomposites which are sheared into photonic crystals at 150 degrees C using a high-pressure quartz-cell multipass rheometer. Broadband spectroscopy of the resonant Bragg scattering peak allows the direct observation of crystal formation and melting of monodisperse core-shell particles. A range of flow conditions of this solventless, highly viscous melt reveals four distinct regimes of crystal growth and decay which match a simple rheological model. Extraction of crystal thickness, order and lattice spacing are validated by one-dimensional electromagnetic simulations.

Strong exciton-photon coupling in inorganic-organic multiple quantum wells embedded low-Q microcavity.

Optoelectronic-compatible heterostructures are fabricated from layered inorganic-organic multiple quantum wells (IO-MQW) of Cyclohexenyl ethyl ammonium lead iodide, (C(6)H(9)C(2)H(4)NH(3))(2)PbI(4) (CHPI). These hybrids possess strongly-resonant optical features, are thermally stable and compatible with hybrid photonics assembly. Room-temperature strong-coupling is observed when these hybrids are straightforwardly embedded in metal-air (M-A) and metal-metal (M-M) low-Q microcavities, due to the large oscillator strength of these IO-MQWs. The strength of the Rabi splitting is 130 meV for M-A and 160 meV for M-M cavities. These values are significantly higher than for J-aggregates in all-metal microcavities of similar length. These experimental results are in good agreement with transfer matrix simulations based on resonant excitons. Incorporating exciton-switching hybrids allows active control of the strong-coupling parameters by temperature, suggesting new device applications.

The fabrication of plasmonic Au nanovoid trench arrays by guided self-assembly.

Metallic nanoscale voids can support both localized and propagating plasmons and form plasmonic crystals. However, constructing 1D arrays is crucial for producing plasmonic circuits. In this paper we report the first experimental evidence of plasmons in templated linear arrays of self-assembled structures. Single and multilayer arrays of gold voids have been fabricated by self-assembly of sub-micron polystyrene spheres in V-shaped trenches in silicon, followed by selective area electrodeposition. Angle-dependent dispersion characteristics reveal the existence of localized plasmons.

UV SERS at well ordered Pd sphere segment void (SSV) nanostructures.

Ultraviolet laser excited surface-enhanced Raman scattering was obtained for the first time at the well ordered palladium sphere segment void (SSV) nanostructures, using adenine as the probe molecule, and the UV-SERS enhancement is found to be correlated well with the plasmon absorption of Pd SSVs in the UV region.