Superfluidity-the suppression of scattering in a quantum fluid at velocities below a critical value-is one of the most striking manifestations of the collective behaviour typical of Bose-Einstein condensates. This phenomenon, akin to superconductivity in metals, has until now only been observed at prohibitively low cryogenic temperatures.For atoms, this limit is imposed by the small thermal de Broglie wavelength, which is inversely related to the particle mass. Even in the case of ultralight quasiparticles such as exciton-polaritons, superfluidity has only been demonstrated at liquid helium temperatures. In this case, the limit is not imposed by the mass, but instead by the small exciton binding energy of Wannier-Mott excitons, which places the upper temperature limit. Here we demonstrate a transition from normal to superfluid flow in an organic microcavity supporting stable Frenkel exciton-polaritons at room temperature. This result paves the way not only to table-top studies of quantum hydrodynamics, but also to room-temperature polariton devices that can be robustly protected from scattering.
Exciton-polaritons are bosonic quasiparticles that arise from the normal mode splitting of photons in a microcavity and excitons in a semiconductor material. One of the most intriguing extensions of such a light−matter interaction is the socalled ultrastrong coupling regime. It is achieved when the Rabi frequency (Ω R , the energy exchange rate between the emitter and the resonant photonic mode) reaches a considerable fraction of the emitter transition frequency, ω 0 . Here, we report a Rabi energy splitting (2ℏΩ R ) of 1.12 eV and record values of the coupling ratio (2Ω R /ω 0 ) up to 0.6-fold the material band gap in organic semiconductor microcavities and up to 0.5-fold in monolithic heterostructure organic light-emitting diodes working at room temperature. Furthermore, we show that with such a large coupling strength it is possible to undress the exciton homogeneous linewidth from its inhomogeneous broadening, which allows for an unprecedented narrow emission line (below the cavity finesse) for such organic LEDs. The latter can be exploited for the realization of novel monochromatic sources and near-IR organic emitting devices.
Evidence of complementary carrier percolation paths in halide perovskite-sensitized mesostructured solar cells.
The strong coupling of an excitonic transition with an electromagnetic mode results in composite quasi-particles called exciton polaritons, which have been shown to combine the best properties of their individual components in semiconductor microcavities. However, the physics and applications of polariton flows in organic materials and at room temperature are still unexplored because of the poor photon confinement in such structures. Here, we demonstrate that polaritons formed by the hybridization of organic excitons with a Bloch surface wave are able to propagate for hundreds of microns showing remarkable third-order nonlinear interactions upon high injection density. These findings pave the way for the study of organic nonlinear light–matter fluxes and for a technologically promising route of the realization of dissipation-less on-chip polariton devices operating at room temperature.
Nanyang Technological University 637371, SingaporeMachine learning software applications are nowadays ubiquitous in many fields of science and society for their outstanding capability of solving computationally vast problems like the recognition of patterns and regularities in big datasets. One of the main goals of research is the realization of a physical neural network able to perform data processing in a much faster and energyefficient way than the state-of-the-art technology. Here we show that lattices of exciton-polariton condensates accomplish neuromorphic computing using fast optical nonlinearities and with lower error rate than any previous hardware implementation. We demonstrate that our neural network significantly increases the recognition efficiency compared to the linear classification algorithms on one of the most widely used benchmarks, the MNIST problem, showing a concrete advantage from the integration of optical systems in reservoir computing architectures.
Excitonic/electronic coupling and cooperative interactions in self-assembled lead halide perovskite nanocrystals were reported to give rise to a collective low energy emission peak with accelerated dynamics. Here we report that similar spectroscopic features could appear as a result of the nanocrystal reactivity within the self-assembled superlattices. This is demonstrated by using CsPbBr3 nanocrystal superlattices under room temperature and cryogenic micro-photoluminescence spectroscopy. It is shown that keeping such structures under vacuum, a gradual contraction of the superlattices and subsequent coalescence of the nanocrystals occurs over several days. As a result, a narrow, low energy emission peak is observed at 4 K with a concomitant shortening of the photoluminescence lifetime due to the energy transfer between nanocrystals. When exposed to air, self-assembled CsPbBr3 nanocrystals develop bulk-like CsPbBr3 particles on top of the superlattices. At 4 K, these particles produce a distribution of narrow, low energy emission peaks with short lifetimes and excitation fluence-dependent, oscillatory decays, resembling the features of superfluorescence. Overall, the reactivity of CsPbBr3 nanocrystals dramatically alters the emission of their assemblies, which should not be overlooked when studying collective optoelectronic properties nor confused with superfluorescence effects.
Abstract.Hybrid composites obtained upon blending conjugated polymers and colloidal semiconductor nanocrystals are regarded as attractive photoactive materials for optoelectronic applications.Here we demonstrate that tailoring nanocrystal surface chemistry permits to control noncovalent and electronic interactions between organic and inorganic components. We show that the pending moieties of organic ligands at the nanocrystal surface do not merely confer colloidal stability while hindering charge separation and transport, but drastically impact morphology of hybrid composites during formation from blend solutions. The relevance of our approach to photovoltaic applications is demonstrated for composites based on poly(3-hexylthiophene) and lead sulfide nanocrystals, considered as inadequate until this report, which enable the fabrication of hybrid solar cells displaying a power conversion efficiency that reaches 3 %. By investigating (quasi)steady-state and time-resolved photo-induced processes in the nanocomposites and their constituents, we ascertain that electron transfer occurs at the hybrid interface yielding long-lived separated charge carriers, whereas interfacial hole transfer appears hindered. Here we provide a reliable alternative aiming to gain control over macroscopic optoelectronic properties of polymer/nanocrystal composites by mediating their non-covalent interactions via ligands' pending moieties, thus opening new possibilities towards efficient solution-processed hybrid solar cells.3
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