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We develop a feedback strategy based on optimal quantum feedback control for Gaussian systems to maximise the likelihood of steady-state entanglement detection between two directly interacting masses. We employ linear quadratic Gaussian (LQG) control to engineer the phase space dynamics of the two masses and propose Einstein-Podolsky-Rosen (EPR)-type variance minimisation constraints for the feedback to facilitate unconditional entanglement generation. This scheme allows for stationary entanglement in parameter regimes where strategies based on total energy minimisation ($cooling$) would fail. This feedback strategy, applied to the system of two masses driven out-of-thermal equilibrium [arXiv:2408.06251] enables unconditional entanglement generation under realistic experimental conditions.

We present a protocol that maximizes unconditional entanglement generation between two masses interacting directly through $1/r^{n}$ potential. The protocol combines optimal quantum control of continuously measured masses with their non-equilibrium dynamics, driven by a time-dependent interaction strength. Applied to a pair of optically trapped sub-micron particles coupled via electrostatic interaction, our protocol enables unconditional entanglement generation at the fundamental limit of the conditional state and with an order of magnitude smaller interaction between the masses compared to the existing steady-state approaches.

The advent of organic polaritonics has led to the realisation of all-optical transistors, logic gates, and single photon-switches operating at room temperature. In this Letter, we develop a microscopic theory accounting for thermalisation, vibron-relaxation, and radiative and ballistic polariton losses to investigate the intrinsic limitations of the temporal separation of consecutive polariton condensates. We test and verify our theoretical predictions using an optical pump-pump configuration with different pulse width and unravel the importance of lateral ballistic losses in defining the upper limit of the temporal bandwidth, reaching ~240 GHz.

In this work, we develop an optomechanical formalism for macroscopic quantum states in exciton-polariton systems with strong exciton-phonon interactions. We show that polariton optomechanical interactions induce dynamical backaction, resulting in dispersive and dissipative shifts in the complex vibrational response functions. Unlike conventional optomechanical systems, polariton optomechanics features high-dimensionality and phase-space confinement due to the dispersion relations of exciton-polaritons. Consequently, vibrational modes exhibit effective positive or negative mass depending on the detuning parameter, and are capable for the nonequilibrium vibrational Bose-Einstein condensation under the resonant conditions [arXiv:2309.08498]. We demonstrate the potential for vibrational control of polariton condensates at room temperature.

Polariton thermalization is a key process in achieving light-matter Bose--Einstein condensation, spanning from solid-state semiconductor microcavities at cryogenic temperatures to surface plasmon nanocavities with molecules at room temperature. Originated from the matter component of polariton states, the microscopic mechanisms of thermalization are closely tied to specific material properties. In this work, we investigate polariton thermalization in strongly-coupled molecular systems. We develop a microscopic theory addressing polariton thermalization through electron-phonon interactions (known as exciton-vibration coupling) with low-energy molecular vibrations. This theory presents a simple analytical method to calculate the temperature-dependent polariton thermalization rate, utilizing experimentally accessible spectral properties of bare molecules, such as the Stokes shift and temperature-dependent linewidth of photoluminescence, in conjunction with well-known parameters of optical cavities. Our findings demonstrate qualitative agreement with recent experimental reports of nonequilibrium polariton condensation in both ground and excited states, and explain the thermalization bottleneck effect observed at low temperatures. This study showcases the significance of vibrational degrees of freedom in polariton condensation and offers practical guidance for future experiments, including the selection of suitable material systems and cavity designs.

We demonstrate a macro-coherent regime in exciton-polariton systems, where nonequilibrium polariton Bose--Einstein condensation coexists with macroscopically occupied vibrational states. Strong exciton-vibration coupling induces an effective optomechanical interaction between cavity polaritons and vibrational degrees of freedom of molecules, leading to vibrational amplification in a resonant blue-detuned configuration. This interaction provide a sympathetic mechanism to achieve vibrational condensation with potential applications in cavity-controlled chemistry, nonlinear and quantum optics.

We investigate active spatial control of polariton condensates independently of the polariton-, gain-inducing excitation profile. This is achieved by introducing an extra intracavity semiconductor layer, non-resonant to the cavity mode. Saturation of the optical absorption in the uncoupled layer enables the ultra-fast modulation of the effective refractive index and, through excited-state absorption, the polariton dissipation. Utilising these mechanisms, we demonstrate control over the spatial profile and density of a polariton condensate at room temperature.

The manipulation of exciton-polaritons and their condensates is of great interest due to their applications in polariton simulators and high-speed, all-optical logic devices. Until now, methods of trapping and manipulating such condensates are not dynamically reconfigurable or result in an undesirable reduction in the exciton-photon coupling strength. Here, we present a new strategy for the ultrafast control of polariton resonances via transient modification of an optical cavity mode. We have constructed multilayer organic semiconductor microcavities that contain two absorbers: one strongly- and one weakly-coupled to the cavity photon mode. By selectively exciting the weakly-coupled absorber with ultrashort laser pulses, we modulate the cavity refractive index and generate fully-reversible blueshifts of the lower polariton branch by up to 8 meV in sub-ps timescales with no corresponding reduction in the exciton-photon coupling strength. Our work demonstrates the ability to manipulate polariton energy landscapes over ultrafast timescales with important applications in emerging computing technologies.

In this letter, we give an analytical quantum description of a non-equilibrium 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 non-equilibrium 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 non-equilibrium 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 polariton condensate drops below the reservoir temperature.

Linear carbon-based materials such as polyyne and cumulene oligomers provide a versatile platform for nano-physics and engineering. Direct gap quasi-1D polyyne structures are promising for the observation of strong and unusual excitonic eects arising due to the two-dimensional quantum connement. Recently, we reported on the observation of sharp exciton peaks in low temperature photoluminescence spectra of polyyne chains. Here, we analyse the time-resolved optical response of this system. We extend the non-local dielectric response theory to predict the exciton radiative lifetime dependence on the band-gap value and on the length of the chain. A good agreement between the experiment and the theory is achieved., Comment: 4 pages, 4 figures

We implement full polarization tomography on the photon correlations in a spinor exciton-polariton condensate. Our measurements reveal condensate pseudospin mean-field dynamics spanning from stochastic switching between linear polarization components, limit cycles, and stable fixed points, and their intrinsic relation to the condensate photon statistics. We optically harness the cavity birefringence, polariton interactions, and the optical orientation of the photoexcited exciton background to engineer photon statistics with precise control. Our results demonstrate a smooth transition from a highly coherent to a super-thermal state of the condensate polarization components.

Recently, we have experimentally observed signatures of sharp exciton peaks in the photoluminescence spectra of bundles of monoatomic carbon chains stabilized by gold nanoparticles and deposited on a glass substrate. Here, we estimate the characteristic energies of excitonic transitions in this complex quasi-one-dimensional nano-system with use of the variational method. We show that the characteristic energy scale for the experimentally observed excitonic fine structure is governed by the interplay between the hopping energy in a Van der Waals quasicrystal formed by parallel carbon chains, the neutral-charged exciton splitting and the positive-negative trion splitting. These three characteristic energies are an order of magnitude lower than the direct exciton binding energy., Comment: 6 pages, 3 figures

Organic semiconductors are a promising platform for ambient polaritonics. Several applications, such as polariton routers, and many-body condensed matter phenomena are currently hindered due to the ultra-short polariton lifetimes in organics. Here, we employ a single-shot dispersion imaging technique, using 4 nanosecond long non-resonant excitation pulses, to study polariton lasing in a $\lambda/2$ planar organic microcavity filled with BODIPY-Br dye molecules. At a power threshold density of $1.5 MW/cm^{2}$, we observe the transition to a quasi-steady state, 1.2 ns long-lived, single-mode polariton lasing and the concomitant superlinear increase of photoluminescence, spectral line-narrowing, and energy blueshift

The recent progress in nanotechnology [1,2] and single-molecule spectroscopy [3-5] paves the way for cost-effective organic quantum optical technologies emergent with a promise to real-life devices operating at ambient conditions. In this letter, we harness $\pi$-conjugated segments of an organic ladder-type polymer strongly coupled to a microcavity forming correlated collective dressed states of light, so-called of exciton-polariton condensates. We explore an efficient way for all-optical ultra-fast control over the macroscopic condensate wavefunction via a single photon. Obeying Bose statistics, exciton-polaritons exhibit an extreme nonlinearity undergoing bosonic stimulation [6] which we have managed to trigger at the single-photon level. Relying on the nature of organic matter to sustain stable excitons dressed with high energy molecular vibrations we have developed a principle that allows for single-photon nonlinearity operation at ambient conditions opening the door for practical implementations like sub-picosecond switching, amplification and all-optical logic at the fundamental limit of single light quanta.

Today, almost all information processing is performed using electronic logic circuits operating with up to several gigahertz frequency. All-optical logic, however, that holds the promise to allow up to three orders of magnitude higher speed [1] has not been able to provide a viable alternative because approaches that had been tried were either not scalable, not energy efficient or did not show a significant speed benefit. Whereas essential all-optical transistor functionalities have been already demonstrated across a range of platforms [2-4], using them to implement the complete Boolean logic gate set and in particular negation - switching off an optical signal with another optical signal - poses a major challenge [5]. Here, we realize a universal NOR logic gate by introducing the concept of non-ground-state dynamic exciton-polariton condensation in an organic semiconductor microcavity under non-resonant pulsed excitation. In the presence of either of the input signals inserted at opposite in-plane momenta, non-ground state dynamic condensation supersedes spontaneous ground-state condensation, resulting in a NOR-operator output signal within less than a picosecond. An additional optical transistor, fed by the output of the NOR gate, is then used to regenerate the output signal such that it is usable as input for cascading gates, a prerequisite for scale up. Our results constitute an essential step towards the realization of more complex logic optical circuitry that could boost future information processing applications.

Coherent bosonic ensembles offer the promise of harnessing quantum effects in photonic and quantum circuits. In the dynamic equilibrium regime, the application of polariton condensates is hindered by exciton-polariton scattering induced de-coherence in the presence of a dark exciton reservoir. By spatially separating the condensate from the reservoir, we drive the system into the weak interaction regime, where the ensemble coherence time exceeds the individual particle lifetime by nearly three orders of magnitude. The observed nanosecond coherence provides an upper limit for polariton self-interactions. In contrast to conventional photon lasers, we observe an increased contribution from the super-Poissonian component of the condensate to the overall particle number fluctuations. Coupled with the recent emergence of a quantum regime in polaritonics, coherence times extended to several nanoseconds favour the realization of quantum information protocols., Comment: 15pages, 4 figures and supplementary information

We studied monoatomic linear carbon chains stabilised 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, 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 non-radiative 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., Comment: 23 pages, 5 figures

We report on the origin of energy-shifts in organic polariton condensates. The localised nature of Frenkel excitons in molecular semiconductors precludes interparticle Coulomb exchange interactions -the latter being the dominant mechanism for blueshifts in inorganic semiconductor microcavities that bear Wannier-Mott excitons. We examine the contribution of optically induced change of the intracavity non-linear refractive index, gain induced frequency-pulling and quenching of the Rabi splitting, as well as the role of polariton-exciton and polariton-polariton scattering in the energy-shift of the polariton mode at condensation threshold in strongly coupled molecular dye microcavities. We conclude that blueshifts in organic polariton condensates arise from the interplay of the saturation of molecular optical transitions and intermolecular energy migration. Our model predicts the commonly observed step-wise increase of both the emission energy and degree of linear polarisation at polariton condensation threshold.

Novel microstamping tool for microarray printing is proposed. The tool is capable to spot up to 127 droplets of different solutions in single touch. It is easily compatible with commercially available microarray spotters. The tool is based on multichannel funnel with polypropylene capillaries inserted into its channels. Superior flexibility is achieved by ability to replace any printing capillary of the tool. As a practical implementation, hydrogel-based microarrays were stamped and successfully applied to identify the Mycobacterium tuberculosis drug resistance.