Hamid Ohadi

Single-molecule optomechanics in “picocavities”

A cool route to nanospectroscopy Confining light to a cavity is often used to enhance the interaction between the light and a particle stored within the cavity. Benz et al. worked with a self-assembled monolayer of biphenyl-4-thiol molecules sandwiched between a gold film and a gold nanoparticle. They used laser irradiation to move atoms in the nanoparticle and produced a “picocavity” that was stable at cryogenic temperatures. The authors were then able to obtain time-dependent Raman spectra from individual molecules. Such subwavelength cavities that can localize light to volumes well below 1 nm3 will enable optical experiments on the atomic scale. Science, this issue p. 726 Strongly subwavelength optical cavities can be used to spectroscopically probe single molecules. Trapping light with noble metal nanostructures overcomes the diffraction limit and can confine light to volumes typically on the order of 30 cubic nanometers. We found that individual atomic features inside the gap of a plasmonic nanoassembly can localize light to volumes well below 1 cubic nanometer (“picocavities”), enabling optical experiments on the atomic scale. These atomic features are dynamically formed and disassembled by laser irradiation. Although unstable at room temperature, picocavities can be stabilized at cryogenic temperatures, allowing single atomic cavities to be probed for many minutes. Unlike traditional optomechanical resonators, such extreme optical confinement yields a factor of 106 enhancement of optomechanical coupling between the picocavity field and vibrations of individual molecular bonds. This work sets the basis for developing nanoscale nonlinear quantum optics on the single-molecule level.

Nonlinear optical spin hall effect and long-range spin transport in polariton lasers

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.

SERS of Individual Nanoparticles on a Mirror: Size Does Matter, but so Does Shape

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.

Polariton condensation in an optically induced two-dimensional potential

We demonstrate experimentally the condensation of exciton polaritons through optical trapping. The nonresonant pump profile is shaped into a ring and projected to a high quality factor microcavity where it forms a two-dimensional 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 buildup 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 much stronger dephasing and depletion processes.

Spontaneous Spin Bifurcations and Ferromagnetic Phase Transitions in a Spinor Exciton-Polariton Condensate

This work was supported by Grants EPSRC No. EP/G060649/1, EU No. CLERMONT4 235114, EU No. INDEX 289968, Spanish MEC (MAT2008-01555), Greek GSRT ARISTEIA Apollo program and Fundacion La Caixa, and Mexican CONACYT No. 251808. FP acknowledges financial support through an EPSRC doctoral prize fellowship at the University of Cambridge and a Schrodinger fellowship at the University of Oxford.

Spontaneous symmetry breaking in a polariton and photon laser.

We report on the simultaneous observation of spontaneous symmetry breaking and long-range spatial coherence both in the strong- and the weak-coupling regime in a semiconductor microcavity. Under pulsed excitation, the formation of a stochastic order parameter is observed in polariton and photon lasing regimes. Single-shot measurements of the Stokes vector of the emission exhibit the buildup of stochastic polarization. Below threshold, the polarization noise does not exceed 10%, while above threshold we observe a total polarization of up to 50% after each excitation pulse, while the polarization averaged over the ensemble of pulses remains nearly zero. In both polariton and photon lasing regimes, the stochastic polarization buildup is accompanied by the buildup of spatial coherence. We find that the Landau criterion of spontaneous symmetry breaking and Penrose-Onsager criterion of long-range order for Bose-Einstein condensation are met in both polariton and photon lasing regimes.

Robust platform for engineering pure-quantum-state transitions in polariton condensates

We report on pure-quantum-state polariton condensates in optical annular traps. The study of the underlying mechanism reveals that the polariton wave function always coalesces in a single pure quantum state that, counter-intuitively, is always the uppermost confined state with the highest overlap with the exciton reservoir. The tunability of such states combined with the short polariton lifetime allows for ultrafast transitions between coherent mesoscopic wave functions of distinctly different symmetries, rendering optically confined polariton condensates a promising platform for applications such as many-body quantum circuitry and continuous-variable quantum processing.

Linear wave dynamics explains observations attributed to dark solitons in a polariton quantum fluid

We investigate the propagation and scattering of polaritons in a planar GaAs microcavity in the linear regime under resonant excitation. The propagation of the coherent polariton wave across an extended defect creates phase and intensity patterns with identical qualitative features previously attributed to dark and half-dark solitons of polaritons. We demonstrate that these features are observed for negligible nonlinearity (i.e., polariton-polariton interaction) and are, therefore, not sufficient to identify dark and half-dark solitons. A linear model based on the Maxwell equations is shown to reproduce the experimental observations.

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.

A sub-femtojoule electrical spin-switch based on optically trapped polariton condensates

Practical challenges to extrapolating Moores 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.