Coinage metal nanostructures support localised surface plasmons, which confine optical fields much tighter than their wavelength (1). This extreme enhancement enables vibrational spectroscopy within small volumes, even down to single molecules (2,3). For many years lateral resolution was believed to be 10 nm (4), however recent experiments resolve the atomic structure of single molecules using tipenhanced Raman spectroscopy (3) and directly sequence RNA strands (5). Atomistic simulations also suggest plasmonic confinement to atomic scales is possible (6). Here we show that light-activated mobilisation of surface atoms in a plasmonic hotspot triggers the formation of additional 'picocavities'bounded by a single gold atom. Their ultra-small light localisation alters which vibrational modes of trapped molecules are observed, due to strong optical field gradients that switch the Raman selection rules. The resulting cascaded ultra-strong plasmonic confinement pumps specific molecular bonds, thereby creating non-thermal vibrational populations, and forms a new type of optomechanical

Coupling noble metal nanoparticles by a 1 nm gap to an underlying gold mirror confines light to extremely small volumes, useful for sensing on the nanoscale. Individually measuring 10 000 of such gold nanoparticles of increasing size dramatically shows the different scaling of their optical scattering (far-field) and surface-enhanced Raman emission (SERS, near-field). Linear red-shifts of the coupled plasmon modes are seen with increasing size, matching theory. The total SERS from the few hundred molecules under each nanoparticle dramatically increases with increasing size. This scaling shows that maximum SERS emission is always produced from the largest nanoparticles, irrespective of tuning to any plasmonic resonances. Changes of particle facet with nanoparticle size result in vastly weaker scaling of the near-field SERS, without much modifying the far-field, and allows simple approaches for optimizing practical sensing.

We report on the experimental observation of the nonlinear analogue of the optical spin Hall effect under highly nonresonant circularly polarized excitation of an exciton-polariton condensate in a GaAs/AlGaAs microcavity. The circularly polarized polariton condensates propagate over macroscopic distances, while the collective condensate spins coherently precess around an effective magnetic field in the sample plane performing up to four complete revolutions.

We observe a spontaneous parity breaking bifurcation to a ferromagnetic state in a spatiallytrapped exciton-polariton condensate. At a critical bifurcation density under nonresonant excitation, the whole condensate spontaneously magnetizes and randomly adopts one of two ellipticallypolarized (up to 95% circularly-polarized) states with opposite handedness of polarization. The magnetized condensate remains stable for many seconds at 5 K, but at higher temperatures it can flip from one magnetic orientation to another. We optically address these states and demonstrate the inversion of the magnetic state by resonantly injecting 100-fold weaker pulses of opposite spin. Theoretically, these phenomena can be well described as spontaneous symmetry breaking of the spin degree of freedom induced by different loss rates of the linear polarizations.Condensation of exciton-polaritons (polaritons) spontaneously breaks the global phase symmetry [1][2][3][4][5]. Owing to their easy optical interrogation, high-speed (ps) interactions, and macroscopic coherence (over hundreds of microns) [6], polariton condensates are excellent candidates to probe and exploit for sensing [7,8], spinoptronics [9][10][11], new optoelectronic devices [12][13][14], and quantum simulators [15]. The driven-dissipative multicomponent polariton system can undergo additional bifurcations and condense into states which are not eigenstates of the single-particle Hamiltonian, but many-body states with reduced symmetry [16,17]. Thus, we should expect that two-component exciton-polariton condensates can also show spontaneous symmetry breaking bifurcations in their polarization state. Spin studies of microcavity polaritons have been of great interest in recent years [18][19][20][21][22][23][24][25][26][27][28][29]. However, spontaneous symmetry-breaking bifurcation of spin has not been observed before.Here, we demonstrate spontaneous magnetization in an exciton-polariton condensate, as a direct result of bifurcations in the spin degree of freedom. Utilizing an optically trapped geometry, condensates spontaneously emerge in either of two discrete spin-polarized states that are stable for many seconds, > 10 10 longer than their formation time. These states emit highly circularly-polarized coherent light (up to 95%) and have opposite circular polarizations. The condensate stochastically condenses in a left-or right-circularly polarized state, with an occurrence likelihood that can be controlled by the ellipticity * ho278@cam.ac.uk † jjb12@cam.ac.uk of the nonresonant pump. The two spin-polarized states can be initialized and switched from one state to another with weak resonant optical pulses. Our system has potential applications in sensing, optical spin memories and spin switches, and it can be implemented for studying long-range spin interactions in polariton condensate lattices. This article is structured as follows: in Section I we review trapped polariton condensates and the current understanding of polarization in untrapped polariton condensates. In Section ...

We demonstrate experimentally the condensation of exciton-polaritons through optical trapping. The non-resonant pump profile is shaped into a ring and projected to a high quality factor microcavity where it forms a 2D repulsive optical potential originating from the interactions of polaritons with the excitonic reservoir. Increasing the population of particles in the trap eventually leads to the emergence of a confined polariton condensate that is spatially decoupled from the decoherence inducing reservoir, before any build up of coherence on the excitation region. In a reference experiment, where the trapping mechanism is switched off by changing the excitation intensity profile, polariton condensation takes place for excitation densities more than two times higher and the resulting condensate is subject to a much stronger dephasing and depletion processes.Strong coupling of cavity photons and quantum-well excitons gives rise to mixed light-matter bosonic quasiparticles called exciton-polaritons or polaritons [1]. Due to their photonic component, polaritons are several orders of magnitude lighter than atoms, which makes their condensation attainable at higher temperatures [2,3]. The manifestations of polariton condensation include polariton lasing [4], long-range spatial coherence [5,6] and stochastic vector polarisation [7]. In an ideal infinite twodimensional cavity the polariton gas is expected to undergo the Berezinsky-Kosterlitz-Thouless (BKT) phase transition [8], while in realistic structures, polaritons can condense in traps induced by random optical disorder [2] or mechanically created potentials [3,9]. Polariton condensation has also been observed in structures of lower dimensionality [10][11][12][13] where the structure itself acts as the trapping potential. Furthermore, the manipulation of polariton condensates by optically generated potentials has been previously shown [14][15][16]. In these works the condensation process was not assisted by the optical potential but used to localize an already formed polariton condensate.Here, we report on the first manifestation of polariton condensation assisted by an optically generated two dimensional potential. This scheme allows for the formation of a polariton condensate spatially separated from the excitation spot. Owing to the efficient trapping in the optical potential we observe a reduced excitation density threshold as well as higher coherence due to the decoupling of the condensate from the exciton reservoir. Polariton condensation prior to the build-up of coherence in the form of photon or polariton lasing [17,18] at the excitation area on the sample, decisively resolves the debate on the phase relation between the excitation laser and polariton condensate.We used a high quality factor GaAs/AlGaAs microcavity containing four separate triplets of 10 nm GaAs quantum wells and has a vacuum Rabi splitting of 9 meV [19], held at ∼ 6.5 K in a cold-finger cryostat and excited non-resonantly at the first reflection minimum above the cavity stop band with a s...

Practical challenges to extrapolating Moore's law favour alternatives to electrons as information carriers. Two promising candidates are spin-based and all-optical architectures, the former offering lower energy consumption, the latter superior signal transfer down to the level of chip-interconnects. Polaritons-spinor quasi-particles composed of semiconductor excitons and microcavity photons-directly couple exciton spins and photon polarizations, combining the advantages of both approaches. However, their implementation for spintronics has been hindered because polariton spins can be manipulated only optically or by strong magnetic fields. Here we use an external electric field to directly control the spin of a polariton condensate, bias-tuning the emission polarization. The nonlinear spin dynamics offers an alternative route to switching, allowing us to realize an electrical spin-switch exhibiting ultralow switching energies below 0.5 fJ. Our results lay the foundation for development of devices based on the electro-optical control of coherent spin ensembles on a chip.

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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.