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Register a new userOn the origin of blueshifts in organic polariton condensates
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Pavlos Lagoudakis Prof
Publication date
2019
fields
Physics
and research's language is
English
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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.
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Interacting Bosons, loaded in artificial lattices, have emerged as a modern platform to explore collective manybody phenomena, quantum phase transitions and exotic phases of matter as well as to enable advanced on chip simulators. Such experiments strongly rely on well-defined shaping the potential landscape of the Bosons, respectively Bosonic quasi-particles, and have been restricted to cryogenic, or even ultra-cold temperatures. On chip, the GaAs-based exciton-polariton platform emerged as a promising system to implement and study bosonic non-linear systems in lattices, yet demanding cryogenic temperatures. In our work, we discuss the first experiment conducted on a polaritonic lattice at ambient conditions: We utilize fluorescent proteins as an excitonic gain material, providing ultra-stable Frenkel excitons. We directly take advantage of their soft nature by mechanically shaping them in the photonic one-dimensional lattice. We demonstrate controlled loading of the condensate in distinct orbital lattice modes of different symmetries, and finally explore, as an illustrative example, the formation of a gap solitonic mode, driven by the interplay of effective interaction and negative effective mass in our lattice. The observed phenomena in our open dissipative system are comprehensively scrutinized by a nonequilibrium model of polariton condensation. We believe, that this work is establishing the organic polariton platform as a serious contender to the well-established GaAs platform for a wide range of applications relying on coherent Bosons in lattices, given its unprecedented flexibility, cost effectiveness and operation temperature.
Observation of quantized vortices in non-equilibrium polariton condensates has been reported either by spontaneous formation and pinning in the presence of disorder or by imprinting them onto the signal or idler of an optical parametric oscillator (OPO). Here, we report a detailed analysis of the creation and annihilation of polariton vortex-antivortex pairs in the signal state of a polariton OPO by means of a short optical Gaussian pulse at a certain finite pump wave-vector. A time-resolved, interferometric analysis of the emission allows us to extract the phase of the perturbed condensate and to reveal the dynamics of the supercurrents created by the pulsed probe. This flow is responsible for the appearance of the topological defects when counter-propagating to the underlying currents of the OPO signal.
The strong light-matter coupling of a microcavity mode to tightly bound Frenkel excitons in organic materials emerged as a versatile, room-temperature compatible platform to study nonlinear many-particle physics and bosonic condensation. However, various aspects of the optical response of Frenkel excitons in this regime remained largely unexplored. Here, we utilize a hemispheric optical cavity filled with the fluorescent protein mCherry to address two important questions in the field of room-temperature polariton condensates. First, combining the high quality factor of the microcavity with a well-defined mode structure allows us to provide a definite answer whether temporal coherence in such systems can become competitive with their low-temperature counterparts. We observe highly monochromatic and coherent light beams emitted from the condensate, characterized by a coherence time greater than 150$,$ps, which exceeds the polariton lifetime by two orders of magnitude. Second, the high quality of our device allows to sensibly trace the emission energy of the condensate, and thus to establish a fundamental picture which quantitatively explains the core nonlinear processes yielding the characteristic density-dependent blueshift. We find that the energy shift of Frenkel exciton-polaritons is largely dominated by the reduction of the Rabi-splitting due to phase space filling effects, which is influenced by the redistribution of polaritons in the system. While our finding of highly coherent condensation at ambient conditions addresses the suitability of organic polaritonics regarding their utilization as highly coherent room temperature polariton lasers, shedding light on the non-linearity is of great benefit towards implementing non-linear devices, optical switches, and lattices based on exciton-polaritons at room temperature.
We examine the photoluminescence of highly-excited exciton-polariton condensates in semiconductor microcavities. Under strong pumping, exciton-polariton condensates have been observed to undergo a lasing transition where strong coupling between the excitons and photons is lost. We discuss an alternative high-density scenario, where the strong coupling is maintained. We find that the photoluminescence smoothly transitions between the lower polariton energy to the cavity photon energy. An intuitive understanding of the change in spectral characteristics is given, as well as differences to the photoluminescence characteristics of the lasing case.
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 4-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 8 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 non-equilibrium spin lattice.
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