Microcavity-polaritons are quasi-particles formed when light and matter excitations couple strongly in cavities that have confinement lengths similar to the wavelength of light. Polariton’s light e↵ective mass, due to the photonic component, in conjunction with their composite boson nature, allows a transition into a macroscopically occupied quantum degenerate state (polariton condensate) for temperatures ranging from 4K up to room temperature. Due to the exciton reservoirs produced under non-resonant excitation and polariton’s strong interparticle interactions (originating from their matter component) potential landscapes for the polaritons can be sculpted with the non-resonant laser beam(s) pumping the system. The work presented in this thesis is specifically concerned with inorganic polariton condensates in optically imprinted potential landscapes. With annular excitation geometries it is possible to form optically trapped polariton condensates, where the condensate is spatially delocalised from the exciton reservoir. Implementing this optical trap geometry, the first all-optical polariton bistability under non-resonant excitation is demonstrated in the spinor of the condensate. Furthermore, the separation from the exciton reservoir results in significant enhancement of the coherence properties. First order coherence times exceeding 1.5ns are demonstrated for the optical trap excitation geometry; whilst excitation regimes where the condensate overlaps the reservoir demonstrate sub 100ps coherence times. For narrow Gaussian excitation geometries, the spatial overlap of the condensate and the reservoir results in polaritons ballistically propagating away from pump with a well defined in-plane wavevector. Utilising this inherent in-plane propagation, two freely expanding polariton condensates (a polariton dyad) are shown to remain coupled, even for separation distances exceeding 100μm. Through an in-depth experimental and theoretical investigation of the polariton dyad, it is determined that it is critically important to account for the finite propagation time of polaritons from one condensate centre to the other (i.e. the coupling is time-delayed). The experimental work in this thesis is then concluded by introducing all-optical polariton band structure engineering. Utilising optically imprinted polariton condensates and their exciton reservoirs to both create and image the band structures. In addition to the experimental results, experimental procedures and analysis techniques, that have been developed and implemented to facilitate the research, are presented.
Microcavity-polaritons are quasi-particles formed when light and matter excitations couple strongly in cavities that have confinement lengths similar to the wavelength of light. Polariton’s light e↵ective mass, due to the photonic component, in conjunction with their composite boson nature, allows a transition into a macroscopically occupied quantum degenerate state (polariton condensate) for temperatures ranging from 4K up to room temperature. Due to the exciton reservoirs produced under non-resonant excitation and polariton’s strong interparticle interactions (originating from their matter component) potential landscapes for the polaritons can be sculpted with the non-resonant laser beam(s) pumping the system. The work presented in this thesis is specifically concerned with inorganic polariton condensates in optically imprinted potential landscapes. With annular excitation geometries it is possible to form optically trapped polariton condensates, where the condensate is spatially delocalised from the exciton reservoir. Implementing this optical trap geometry, the first all-optical polariton bistability under non-resonant excitation is demonstrated in the spinor of the condensate. Furthermore, the separation from the exciton reservoir results in significant enhancement of the coherence properties. First order coherence times exceeding 1.5ns are demonstrated for the optical trap excitation geometry; whilst excitation regimes where the condensate overlaps the reservoir demonstrate sub 100ps coherence times. For narrow Gaussian excitation geometries, the spatial overlap of the condensate and the reservoir results in polaritons ballistically propagating away from pump with a well defined in-plane wavevector. Utilising this inherent in-plane propagation, two freely expanding polariton condensates (a polariton dyad) are shown to remain coupled, even for separation distances exceeding 100μm. Through an in-depth experimental and theoretical investigation of the polariton dyad, it is determined that it is critically important to account for the finite propagation time of polaritons from one condensate centre to the other (i.e. the coupling is time-delayed). The experimental work in this thesis is then concluded by introducing all-optical polariton band structure engineering. Utilising optically imprinted polariton condensates and their exciton reservoirs to both create and image the band structures. In addition to the experimental results, experimental procedures and analysis techniques, that have been developed and implemented to facilitate the research, are presented.
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the high energy shift of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that affect nonlinear dynamics and change mechanisms of polariton energy shifts accordingly. We have scrutinized the origins of energy shifts in connection with nonlinear dynamics in Frenkel exciton-polariton condensates and examined the possible contributions: intracavity optical Kerr-effect, gain-induced frequency pulling, polariton interactions and effects related to saturation of optical transitions for "dark"- and "bright" molecules [1]. Unlike the conventional strongly coupled semiconductor microcavities, we have shown that nonlinear interactions within the condensate do not rely on polariton interactions but instead originated from Pauli-blocking principle forbidding double excitation of the same molecular states. We have developed a theoretical model explaining the omnipresent energy shift of the condensate wavefunction together with its spectral and polarization features at the BEC transition in a consistent way. The crucial role of intermolecular energy transfer and “dark” exciton reservoir has been demonstrated for the first time. We believe the principles explored in this work are relevant to other systems exhibiting strong coupling of Frenkel excitons with a cavity mode, regardless of a cavity type, whether one dealing with Fabry-Perot cavities or plasmonic nanocavities etc and; therefore, provide general insight on nonlinear phenomena in composite light-matter condensates. [1] T. Yagafarov, D. Sannikov, A. Zasedatelev, K. Georgiou, A. Baranikov, O. Kyriienko, I. Shelykh, L. Gai, Z. Shen, D. G. Lidzey, P. Lagoudakis, Mechanisms of blueshifts in organic polariton condensates, Commun Phys 3, 18 (2020). https://doi.org/10.1038/s42005-019-0278-6
Condensation of bosons causes spectacular phenomena such as superfluidity or superconductivity. Understanding the nature of the condensed particles is crucial for active control of such quantum phases. Fascinating possibilities emerge from condensates of light–matter-coupled excitations, such as exciton–polaritons, photons hybridized with hydrogen-like bound electron–hole pairs. So far, only the photon component has been resolved, while even the mere existence of excitons in the condensed regime has been challenged. Here we trace the matter component of polariton condensates by monitoring intra-excitonic terahertz transitions. We study how a reservoir of optically dark excitons forms and feeds the degenerate state. Unlike atomic gases, the atom-like transition in excitons is dramatically renormalized on macroscopic ground state population. Our results establish fundamental differences between polariton condensation and photon lasing and open possibilities for coherent control of condensates. Exciton–polaritons are bosonic quasi-particles resulting from strong coupling of excitons and photons but so far only their photon component had been resolved. Here, Menard et al. monitor the intra-excitonic transitions and study how a reservoir of optically dark excitons forms and feeds the degenerate state.
Exciton-polariton Bose-Einstein condensates (BECs) are newly emerged quantum systems that are capable of showing macroscopic quantum phenomena with intrinsic open-dissipative nature. The spatial distribution of the polariton density, without any external potential, can be controlled by the geometric shape of the pumping laser, enabling the investigation of polariton dynamics with topologically non-trivial configurations. Meanwhile, exciton-polaritons have spin degrees of freedom inherited from excitons and photons, making it a candidate for the realization of quantum logic gates. In this thesis, we will investigate theoretically the nonlinear dynamics of exciton-polariton BECs involving both polaritons' spatial degrees of freedom and spin degrees of freedom, and interactions between them. This thesis is organised as follows: In Chapter 1, we will present an overall review of exiton-polariton systems and important properties of polariton BECs and then introduce the dynamical equations with various interactions that will serve as the main theoretical tool for subsequent chapters. Several polariton pumping and trapping techniques appearing in later chapters will also be introduced. In Chapter 2, we will investigate the superfluidity properties of a single-component polariton condensate under an incoherent annular pumping configuration. By studying the stability properties of polariton persistent currents, we find that the persistent currents can exhibit dynamical instability and energetic-like instability according to different parameter region. A stability phase diagram will be given and its relation with the Landau's criterion will be discussed. In Chapter 3, we will investigate the spin dynamics of a two-component polariton condensate under a homogeneous pumping configuration. Owing to the Josephson coupling, there exist multiple steady state solutions that allow of controlled spin state switching. A desynchronized region where there exists no stable steady solution is found. In the desynchronized region, a desynchronized state beating periodically over time can exist, which will serve as a building block of spin waves presented in the next chapter. In Chapter 4, by combining results from the previous two chapters we will investigate generally the nonlinear dynamics of polariton condensates under an annular pumping configuration. The spin-orbit interaction provided by the Josephson coupling supports azimuthon states that have simultaneous modulations in both amplitude and phase. The azimuthon states, when viewed in a different polarization basis, form rotating spin waves that can be referred to as the optical ferris wheel. In Chapter 5, results from previous chapters will be extended to micocavities that support the anisotropic TE-TM splitting interaction. Rotating singularities (small-scale vortices) are found as a result. Their properties and experimental observation techniques will be discussed. Chapter 2-5 provide a theoretical framework for the nonlinear dynamics of polariton condensates. They rely mostly on optical trapping techniques and are ready to be tested in experiments. In Chapter 6, polaritons trapped by an engineered periodic mesa potential will be discussed. We will investigate the band structure of polaritons under the influence of the periodic potential together with discussions on the phase-modulated interference pattern which corresponds to the polariton Talbot patterns observed in experiments.
A bosonic condensate of exciton polaritons in a semiconductor microcavity is a macroscopic quantum state subject to pumping and decay. The fundamental nature of this driven-dissipative condensate is still under debate. Here, we gain an insight into spontaneous condensation by imaging long-lifetime exciton polaritons in a high-quality inorganic microcavity in a single-shot optical excitation regime, without averaging over multiple condensate realisations. We demonstrate that condensation is strongly influenced by an incoherent reservoir and that the reservoir depletion, the so-called spatial hole burning, is critical for the transition to the ground state. Condensates of photon-like polaritons exhibit strong shot-to-shot fluctuations and density filamentation due to the effective self-focusing associated with the reservoir depletion. In contrast, condensates of exciton-like polaritons display smoother spatial density distributions and are second-order coherent. Our observations show that the single-shot measurements offer a unique opportunity to study fundamental properties of non-equilibrium condensation in the presence of a reservoir.
Bose-Einstein condensate of exciton polaritons in a semiconductor microcavity is a macroscopically populated coherent quantum state subject to concurrent pumping and decay. Debates about the fundamental nature of the condensed phase in this open quantum system still persist. Here, we gain a new insight into the spontaneous condensation process by imaging long-lifetime exciton polaritons in a high-quality inorganic microcavity in the single-shot optical excitation regime, without averaging over multiple condensate realisations. In this highly non-stationary regime, a condensate is strongly influenced by the `hot' incoherent reservoir, and reservoir depletion is critical for the transition to the ground energy and momentum state. Condensates formed by more photonic exciton polaritons exhibit dramatic reservoir-induced density filamentation and shot-to-shot fluctuations. In contrast, condensates of more excitonic quasiparticles display smooth density and are second-order coherent. Our observations show that the single-shot measurements offer a unique opportunity to study formation of macroscopic phase coherence during a quantum phase transition in a solid state system.
This thesis includes theoretical studies regarding stability and manipulation of Bose-Einstein condensates (BECs) of ultra-cold atoms in 2D trapping geometry, as well as formation of steady states of exciton-polariton Bose-Einstein condensates created in solid states. We analyze and numerically model the dynamics and localization of the condensates using mean-field model. Chapter 1 contains an introduction to the physics of ultra-cold atom BEC and excitonpolariton BEC which provides a framework for the work presented in later chapters. In Chapter 2, we consider a method for achieving dynamically controllable transport of highly mobile matter-wave solitons in an ultra-cold atom BEC with attractive interparticle interaction loaded into a driven two-dimensional optical lattice. Our numerical analysis based on the mean-field model and the theory based on the effective particle approach demonstrate that fast, time-periodic rocking of the two-dimensional optical lattice enables efficient stabilization and manipulation of spatially localized matter wave packets via induced reconfigurable mobility channels. Chapter 3 consists of an investigation of the instability - collapse of a BEC with attractive interactions. In this chapter we explore the influence of an orbital angular momentum on the collapse of vortex-free elliptic clouds of Bose-Einstein condensates trapped in a radially symmetric harmonic potential or a rotating elliptic potential. The results of our analysis show that the number of trapped ultracold atoms corresponding to the collapse threshold can be radically increased for such rotating nonlinear matter waves in a radially harmonic trap. The results corresponding to a BEC cloud confined in a rotating elliptic trap show that the elongated stationary states can be parallel or perpendicular to the long axis of the trap and display bistable nature. In Chapter 4, we examine spatial localization and dynamical stability of Bose-Einstein condensates of exciton-polaritons in microcavities under the condition of off-resonant spatially inhomogeneous optical pumping both with and without a harmonic trapping potential. We employ the open-dissipative Gross-Pitaevskii model for describing an incoherently pumped polariton condensate coupled to an exciton reservoir. We reveal that spatial localization of the steady-state condensate occurs due to effective self-trapping created by the polariton flows, regardless of the presence of the external potential. A ground state of the polariton condensate with repulsive interactions between the quasiparticles represents a dynamically stable bright dissipative soliton. We also investigate the conditions for sustaining spatially localized structures, with nonzero angular momentum, in the form of single-charge vortices. Chapter 5 consider the existence of novel spatially localized states of exciton-polariton Bose-Einstein condensates in semiconductor microcavities with fabricated periodic inplane potentials. Our theory shows that, under the conditions of continuous nonresonant pumping, localization is observed for a wide range of optical pump parameters due to effective potentials self-induced by the polariton flows in the spatially periodic system. We show that the self-localization of exciton-polaritons in the lattice may occur both in the gaps and bands of the single-particle linear spectrum, and is dominated by the effects of gain and dissipation rather than the structured potential, in sharp contrast to the conservative condensates of ultra-cold alkali atoms.