Single-photon nonlinearity at room temperature.

The recent progress in nanotechnology1,2 and single-molecule spectroscopy3-5 paves the way for emergent cost-effective organic quantum optical technologies with potential applications in useful devices operating at ambient conditions. We harness a π-conjugated ladder-type polymer strongly coupled to a microcavity forming hybrid light-matter states, so-called exciton-polaritons, to create exciton-polariton condensates with quantum fluid properties. Obeying Bose statistics, exciton-polaritons exhibit an extreme nonlinearity when undergoing bosonic stimulation6, which we have managed to trigger at the single-photon level, thereby providing an efficient way for all-optical ultrafast control over the macroscopic condensate wavefunction. Here, we utilize stable excitons dressed with high-energy molecular vibrations, allowing for single-photon nonlinear operation at ambient conditions. This opens new horizons for practical implementations like sub-picosecond switching, amplification and all-optical logic at the fundamental quantum limit.

Controlling the Spatial Profile and Energy Landscape of Organic Polariton Condensates in Double-Dye Cavities.

The development of high-speed, all-optical polariton logic devices underlies emerging unconventional computing technologies and relies on advancing techniques to reversibly manipulate the spatial extent and energy of polartion condensates. We investigate active spatial control of polariton condensates independent of the polariton, gain-inducing excitation profile. This is achieved by introducing an extra intracavity semiconductor layer, nonresonant to the cavity mode. Partial saturation of the optical absorption in the uncoupled layer enables the ultrafast modulation of the effective refractive index and, through excited-state absorption, the polariton dissipation. Utilizing an intricate interplay of these mechanisms, we demonstrate control over the spatial profile, density, and energy of a polariton condensate at room temperature.

Quasiperiodic light.

Quasiperiodicity is a form of spatial order that has been observed in quasicrystalline matter but not light. We construct a quasicrystalline surface out of a light emitting diode. Using a nanoscale waveguide as a microscope (NSOM), we directly image the light field at the surface of the diode. Here we show, using reciprocal space representations of the images, that the light field is quasiperiodic. We explain the structure of the light field with wave superposition. Periodic ordering is limited to at most six-fold symmetry. The light field exhibits 12-fold quasisymmetry, showing order while disproving periodicity. This demonstrates that a new class, consisting of projections from hyperspace, exists in the taxonomy of light ordering.

Spontaneous Formation of Time-Periodic Vortex Cluster in Nonlinear Fluids of Light.

We demonstrate spontaneous formation of a nonlinear vortex cluster state in a microcavity exciton-polariton condensate with time-periodic sign flipping of its topological charges at the GHz scale. When optically pumped with a ring-shaped nonresonant laser, the trapped condensate experiences intricate high-order mode competition and fractures into two distinct trap levels. The resulting mode interference leads to robust condensate density beatings with periodic appearance of orderly arranged phase singularities. Our work opens new perspectives on creating structured free-evolving light, and singular optics in the strong light-matter coupling regime.

Exact Analytical Solution for the Density Matrix of a Nonequilibrium Polariton Bose-Einstein Condensate.

In this Letter, we give an analytical quantum description of a nonequilibrium polariton Bose-Einstein condensate (BEC) based on the solution of the master equation for the full polariton density matrix in the limit of fast thermalization. We find the density matrix of a nonequilibrium BEC, that takes into account quantum correlations between all polariton states. We show that the formation of BEC is accompanied by the build-up of cross-correlations between the ground state and the excited states reaching their highest values at the condensation threshold. Despite the nonequilibrium nature of polariton systems, we show the average population of polariton states exhibits the Bose-Einstein distribution with an almost zero effective chemical potential above the condensation threshold similar to an equilibrium BEC. We demonstrate that above threshold the effective temperature of polaritons drops below the reservoir temperature.

Realizing Optical Persistent Spin Helix and Stern-Gerlach Deflection in an Anisotropic Liquid Crystal Microcavity.

Spin-orbit interactions which couple the spin of a particle with its momentum degrees of freedom lie at the center of spintronic applications. Of special interest in semiconductor physics are Rashba and Dresselhaus spin-orbit coupling. When equal in strength, the Rashba and Dresselhaus fields result in SU(2) spin rotation symmetry and emergence of the persistent spin helix only investigated for charge carriers in semiconductor quantum wells. Recently, a synthetic Rashba-Dresselhaus Hamiltonian was shown to describe cavity photons confined in a microcavity filled with optically anisotropic liquid crystal. In this Letter, we present a purely optical realization of two types of spin patterns corresponding to the persistent spin helix and the Stern-Gerlach experiment in such a cavity. We show how the symmetry of the Hamiltonian results in spatial oscillations of the spin orientation of photons traveling in the plane of the cavity.

Excitonic Fine Structure in Emission of Linear Carbon Chains.

We studied monatomic linear carbon chains stabilized by gold nanoparticles attached to their ends and deposited on a solid substrate. We observe spectral features of straight chains containing from 8 to 24 atoms. Low-temperature PL spectra reveal characteristic triplet fine structures that repeat themselves for carbon chains of different lengths. The triplet is invariably composed of a sharp intense peak accompanied by two broader satellites situated 15 and 40 meV below the main peak. We interpret these resonances as an edge-state neutral exciton and positively and negatively charged trions, respectively. The time-resolved PL shows that the radiative lifetime of the observed quasiparticles is about 1 ns, and it increases with the increase of the length of the chain. At high temperatures a nonradiative exciton decay channel appears due to the thermal hopping of carriers between parallel carbon chains. Excitons in carbon chains possess large oscillator strengths and extremely low inhomogeneous broadenings.

Realizing the classical XY Hamiltonian in polariton simulators.

The vast majority of real-life optimization problems with a large number of degrees of freedom are intractable by classical computers, since their complexity grows exponentially fast with the number of variables. Many of these problems can be mapped into classical spin models, such as the Ising, the XY or the Heisenberg models, so that optimization problems are reduced to finding the global minimum of spin models. Here, we propose and investigate the potential of polariton graphs as an efficient analogue simulator for finding the global minimum of the XY model. By imprinting polariton condensate lattices of bespoke geometries we show that we can engineer various coupling strengths between the lattice sites and read out the result of the global minimization through the relative phases. Besides solving optimization problems, polariton graphs can simulate a large variety of systems undergoing the U(1) symmetry-breaking transition. We realize various magnetic phases, such as ferromagnetic, anti-ferromagnetic, and frustrated spin configurations on a linear chain, the unit cells of square and triangular lattices, a disordered graph, and demonstrate the potential for size scalability on an extended square lattice of 45 coherently coupled polariton condensates. Our results provide a route to study unconventional superfluids, spin liquids, Berezinskii-Kosterlitz-Thouless phase transition, and classical magnetism, among the many systems that are described by the XY Hamiltonian.

Collective Optomechanical Effects in Cavity Quantum Electrodynamics.

We investigate a cavity quantum electrodynamic effect, where the alignment of two-dimensional freely rotating optical dipoles is driven by their collective coupling to the cavity field. By exploiting the formal equivalence of a set of rotating dipoles with a polymer we calculate the partition function of the coupled light-matter system and demonstrate that it exhibits a second order phase transition between a bunched state of isotropic orientations and a stretched one with all the dipoles aligned. Such a transition manifests itself as an intensity-dependent shift of the polariton mode resonance. Our work, lying at the crossroad between cavity quantum electrodynamics and quantum optomechanics, is a step forward in the ongoing quest to understand how strong coupling can be exploited to influence matter internal degrees of freedom.

Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity.

Strongly coupled optical microcavities containing different exciton states permit the creation of hybrid-polariton modes that can be described in terms of a linear admixture of cavity-photon and the constituent excitons. Such hybrid states have been predicted to have optical properties that are different from their constituent parts, making them a test bed for the exploration of light-matter coupling. Here, we use strong coupling in an optical microcavity to mix the electronic transitions of two J-aggregated molecular dyes and use both non-resonant photoluminescence emission and photoluminescence excitation spectroscopy to show that hybrid-polariton states act as an efficient and ultrafast energy-transfer pathway between the two exciton states. We argue that this type of structure may act as a model system to study energy-transfer processes in biological light-harvesting complexes.

Room temperature, cascadable, all-optical polariton universal gates.

Today, almost all information processing is performed using electronic logic circuits operating at several gigahertz frequency. All-optical logic holds the promise to allow for up to three orders of magnitude higher speed. Whereas essential all-optical transistor functionalities were demonstrated across a range of platforms, utilising them to implement a complete Boolean logic gate set and in particular negation, i.e. switching off an optical signal with another, weaker, optical signal, poses a major challenge. Here, we realize a cascadable NOT gate by introducing the concept of non-ground-state polariton amplification in organic semiconductor microcavities under non-resonant optical excitation. We unravel the importance of vibron-mediated stimulated scattering in room temperature operation of the inverter. Moreover, we extend the concept to a multi-input universal NOR logic gate, where in the presence of any of the input signals non-ground-state amplification supersedes spontaneous ground-state condensation, resulting in a NOR gate with ~1 ps switching time. The realisation of an ultrafast universal logic gate constitutes an essential step for more complex optical circuitry that could boost information processing applications.

Laser-Synthesized 2D-MoS2 Nanostructured Photoconductors.

The direct laser synthesis of periodically nanostructured 2D transition metal dichalcogenide (2D-TMD) films, from single source precursors, is presented here. Laser synthesis of MoS2 and WS2 tracks is achieved by localized thermal dissociation of Mo and W thiosalts, caused by the strong absorption of continuous wave (c.w.) visible laser radiation by the precursor film. Moreover, within a range of irradiation conditions we have observed occurrence of 1D and 2D spontaneous periodic modulation in the thickness of the laser-synthesized TMD films, which in some cases is so extreme that it results in the formation of isolated nanoribbons with a width of ~200 nm and a length of several micrometers. The formation of these nanostructures is attributed to the effect that is known as laser-induced periodic surface structures (LIPSS), which is caused by self-organized modulation of the incident laser intensity distribution due to optical feedback from surface roughness. We have fabricated two terminal photoconductive detectors based on nanostructured and continuous films and we show that the nanostructured TMD films exhibit enhanced photo-response, with photocurrent yield increased by three orders of magnitude as compared to their continuous counterparts.

Tunable, continuous-wave Ti:sapphire channel waveguide lasers written by femtosecond and picosecond laser pulses.

Fabrication and cw lasing at 798.25 nm is reported for femtosecond (fs) and picosecond (ps) laser-inscribed channel waveguides in Ti:sapphire crystals. Lasing in channels written by fs (ps) pulses was obtained above a threshold of 84 mW (189 mW) with a maximum output power and a slope efficiency of 143 mW (45 mW) and 23.5% (7.1%), respectively. The emission wavelength was tuned over a 170 nm range by using a birefringent filter in an external cavity.

Electrically tunable Berry curvature and strong light-matter coupling in liquid crystal microcavities with 2D perovskite.

The field of spinoptronics is underpinned by good control over photonic spin-orbit coupling in devices that have strong optical nonlinearities. Such devices might hold the key to a new era of optoelectronics where momentum and polarization degrees of freedom of light are interwoven and interfaced with electronics. However, manipulating photons through electrical means is a daunting task given their charge neutrality. In this work, we present electrically tunable microcavity exciton-polariton resonances in a Rashba-Dresselhaus spin-orbit coupling field. We show that different spin-orbit coupling fields and the reduced cavity symmetry lead to tunable formation of the Berry curvature, the hallmark of quantum geometrical effects. For this, we have implemented an architecture of a photonic structure with a two-dimensional perovskite layer incorporated into a microcavity filled with nematic liquid crystal. Our work interfaces spinoptronic devices with electronics by combining electrical control over both the strong light-matter coupling conditions and artificial gauge fields.

Gauging the flexibility of fluorescent markers for the interpretation of fluorescence resonance energy transfer.

Intramolecular distances in proteins and other biomolecules can be studied in living cells by means of fluorescence resonance energy transfer (FRET) in steady-state or pulsed-excitation experiments. The major uncertainty originates from the unknown orientation between the optical dipole moments of the fluorescent markers, especially when the molecule undergoes thermal fluctuations in physiological conditions. We introduce a statistical method based on the von Mises-Fisher distribution for the interpretation of fluorescence decay dynamics in donor-acceptor FRET pairs that allows us to retrieve both the orientation and the extent of directional fluctuations of the involved dipole moments. We verify the method by applying it to donor-acceptor pairs controllably attached to DNA helices and find that common assumptions such as complete rotational freedom or fully hindered rotation of the dipoles fail a physical interpretation of the fluorescence decay dynamics. This methodology is applicable in single-molecule and ensemble measurements of FRET to derive more accurate distance estimates from optical experiments, without the need for more complex and expensive NMR studies.

Broadband stimulated four-wave parametric conversion on a tantalum pentoxide photonic chip.

We exploit the large third order nonlinear susceptibility (χ(3) or "Chi 3") of tantalum pentoxide (Ta(2)O(5)) planar waveguides and realize broadband optical parametric conversion on-chip. We use a co-linear pump-probe configuration and observe stimulated four wave parametric conversion when seeding either in the visible or the infrared. Pumping at 800 nm we observe parametric conversion over a broad spectral range with the parametric idler output spanning from 1200 nm to 1600 nm in infrared wavelengths and from 555 nm to 600 nm in visible wavelengths. Our demonstration of on-chip stimulated four wave parametric conversion introduces Ta(2)O(5) as a novel material for broadband integrated nonlinear photonic circuit applications.

Optical analogue of the spin Hall effect in a photonic cavity.

We observe anisotropy in the polarization flux generated in a GaAs/AlAs photonic cavity by optical illumination, equivalent to spin currents in strongly coupled microcavities. Polarization rotation of the scattered photons around the Rayleigh ring is due to the TE-TM splitting of the cavity mode. Resolving the circular polarization components of the transmission reveals a separation of the polarization flux in momentum space. These observations constitute the optical analogue of the spin Hall effect.

Dependence of resonance energy transfer on exciton dimensionality.

We investigate the dependence of resonance energy transfer from Wannier-Mott excitons to an organic overlayer on exciton dimensionality. We exploit the excitonic potential disorder in a single quantum well to tune the balance between localized and free excitons by scaling the Boltzmann distribution of excitons through temperature. Theoretical calculations predict the experimentally observed temperature dependence of resonance energy transfer and allow us to quantify the contribution of localized and free excitons. We show that free excitons can undergo resonance energy transfer with an order of magnitude higher rate compared to localized excitons, emphasizing the potential of hybrid optoelectronic devices utilizing resonance energy transfer as a means to overcome charge transfer related limitations.

Geometric frustration in polygons of polariton condensates creating vortices of varying topological charge.

Vorticity is a key ingredient to a broad variety of fluid phenomena, and its quantised version is considered to be the hallmark of superfluidity. Circulating flows that correspond to vortices of a large topological charge, termed giant vortices, are notoriously difficult to realise and even when externally imprinted, they are unstable, breaking into many vortices of a single charge. In spite of many theoretical proposals on the formation and stabilisation of giant vortices in ultra-cold atomic Bose-Einstein condensates and other superfluid systems, their experimental realisation remains elusive. Polariton condensates stand out from other superfluid systems due to their particularly strong interparticle interactions combined with their non-equilibrium nature, and as such provide an alternative testbed for the study of vortices. Here, we non-resonantly excite an odd number of polariton condensates at the vertices of a regular polygon and we observe the formation of a stable discrete vortex state with a large topological charge as a consequence of antibonding frustration between nearest neighbouring condensates.