Observation of two thresholds leading to polariton condensation in 2D hybrid perovskites
Laura Polimeno, Antonio Fieramosca, Giovanni Lerario, Marco Cinquino, Milena De Giorgi, Dario Ballarini, Francesco Todisco, Lorenzo Dominici, Vincenzo Ardizzone… 展开作者
Laura Polimeno, Antonio Fieramosca, Giovanni Lerario, Marco Cinquino, Milena De Giorgi, Dario Ballarini, Francesco Todisco, Lorenzo Dominici, Vincenzo Ardizzone, Marco Pugliese, Carmela T. Prontera, Vincenzo Maiorano, Giuseppe Gigli, Luisa De Marco, Daniele Sanvitto
Two dimensional (2D) perovskites are promising materials for photonic applications, given their outstanding nonlinear optical properties, ease of fabrication and versatility. In particular, exploiting their high oscillator strength, the crystalline form of 2D perovskites can be used as excitonic medium in optical microcavities, allowing for the study of their optical properties in the strong light-matter coupling regime. While polariton condensation has been observed in different materials at room temperature, here we observe for the first time two distinct threshold processes in a 2D perovskite, a material that has never shown spontaneous phase transition up to now. In particular, we demonstrate lasing from the bi-exciton state which contributes to populate the lower polariton branch and, at higher excitation powers, eventually leads to the formation of a polariton condensate. The emission linewidth narrowing and a spatial coherence over 50 x 50 um2 area are the smoking gun, the formation of a quantum coherent state in 2D hybrid perovskite. Our results not only show the formation of a polariton condensate in 2D perovskites but they are also crucial for the understanding of the physical mechanisms that leads to coherent phase transition in perovskite-based polariton microcavities.
Hybrid halide perovskites are now considered as low-cost materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining low-cost devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of the 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton-photon coupling with 3D bromide hybrid perovskite. Cavity polaritons ar…
Strong light-matter interaction enriches topological photonics by dressing light with matter, which provides the possibility to realize tuneable topological devices with immunity to defects. Topological exciton polaritons, half-light half-matter quasiparticles with giant optical nonlinearity represent a unique platform for active topological photonics with phase tunability. Previous demonstrations of exciton polariton topological insulators still demand cryogenic temperatures and their topological properties are usually fixed without phase tunability. Here, we experimentally demonstrate a room…
Optically reconfigurable canalization of exciton-polaritons in a non-hyperbolic perovskite
Nanyang Technological University（南洋理工大学）；B. Verkin Institute for Low Temperature Physics and Engineering of the National Academy of Sciences of Ukraine（乌克兰国家科学院B.维尔金低温物理与工程研究所）；Institut Universitaire de France (IUF)（法兰西学院）；National University of Singapore（新加坡国立大学）
Exciton-polaritons resulting from the strong exciton-photon interaction stimulate the development of novel coherent light sources with low threshold, long range spatial, and temporal coherence to circumvent the ever increasing energy demands of optical communications. Polaritons from bound states in the continuum (BICs) are promising for Bose-Einstein condensation owing to their infinite quality factors that enlarge photon lifetimes and benefit polariton accumulations. However, BIC polariton condensation remains limited to cryogenic temperatures ascribed to the small exciton binding energies o…
Bose-Einstein condensation in strongly correlated lattices provides the possibility to coherently generate macroscopic quantum states, which have attracted tremendous attention as ideal platforms for quantum simulation. Ultracold atoms in optical lattices are one of such promising systems, where their realizations of different phases of matter exhibit promising applications in condensed matter physics, chemistry, and cosmology. Nevertheless, this is only accessible with ultralow temperatures in the nano to micro Kelvin scale set by the typical inverse mass of an atom. Alternative systems such …
Exciton-polaritons in semiconductor microcavities generate fascinating effects such as long-range spatial coherence and Bose-Einstein Condensation (BEC), which are attractive for their potential use in low threshold lasers, vortices and slowing light, etc. However, currently most of exciton-polariton effects either occur at cryogenic temperature or rely on expensive cavity fabrication procedures. Further exploring new semiconductor microcavities with stronger exciton photon interaction strength is extensively needed. Herein, we demonstrate room temperature photon exciton strong coupling in hyb…
Exciton-polaritons, elementary excitations arising from the strong coupling regime between photons and excitons in insulators or semiconductors, represent a promising platform for studying quantum fluids of light and realizing prospective all-optical devices. Among different materials for room temperature polaritonic devices, two-dimensional (2D) layered perovskites have recently emerged as one of the promising candidates thanks to their prominent excitonic features at room temperature. Here we report on the experimental demonstration of exciton-polaritons at room temperature in resonant metas…
We present a microcavity structure with a shifted photonic stop-band to enable efficient non-resonant injection of a polariton condensate with spectrally broad femtosecond pulses. The concept is demonstrated theoretically and confirmed experimentally for a planar GaAs/AlGaAs multilayer heterostructure pumped with ultrashort near-infrared pulses while photoluminescence is collected to monitor the optically injected polariton density. As the excitation wavelength is scanned, a regime of polariton condensation can be reached in our structure at a consistently lower fluence threshold than in a sta…
We demonstrate condensation of microcavity polaritons with a very sharp threshold occuring at two orders of magnitude lower pump intensity than previous demonstrations of condensation. The long cavity-lifetime and trapping and pumping geometries are crucial to the realization of this low threshold. Polariton condensation, or "polariton lasing" has long been proposed as a promising source of coherent light at lower threshold than traditional lasing, and these results suggest methods to bring this threshold even lower.
Polariton lattice condensates provide a platform for on chip quantum emulations. Interactions in extended polariton lattices are currently limited by the intrinsic photonic disorder of microcavities. Here, we fabricate a strain compensated planar GaAs/AlAs microcavity with embedded InGaAs quantum wells and report on polariton condensation under non-resonant optical excitation. Evidence of polariton condensation is supported spectroscopically both in reflection and transmission geometry, whilst the observation of a second threshold to photon lasing allows us to conclusively distinguish between …
Polaritonic devices exploit the coherent coupling between excitonic and photonic degrees of freedom to perform highly nonlinear operations with low input powers. Most of the current results exploit excitons in epitaxially grown quantum wells and require low temperature operation, while viable alternatives have yet to be found at room temperature. Here we show that large single-crystal flakes of two-dimensional layered perovskite are able to sustain strong polariton nonlinearities at room temperature with no need to be embedded in an optical cavity. In particular, exciton-exciton interaction en…
Reconfigurable ultrafast perovskite polariton logic gates via nonlinear dynamics
Peking University（北京大学）；National Center for Nanoscience and Technology（国家纳米科学中心）；University of Chinese Academy of Sciences（中国科学院大学）；Xi'an Jiaotong University（西安交通大学）；Nanyang Technological University（南洋理工大学）；Paderborn University（帕德博恩大学）
Room-temperature cavity exciton-polariton condensation in perovskite quantum dots
IBM Research Europe – Zurich（IBM欧洲苏黎世研究中心）；ETH Zurich（苏黎世联邦理工学院）；Institute of Materials Science of Sevilla, Consejo Superior de Investigaciones Científicas − Universidad de Sevilla (CSIC-US)（塞维利亚材料科学研究所，西班牙国家研究委员会-塞维利亚大学）；Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich（苏黎世联邦理工学院化学与应用生物科学学院无机化学实验室）；Empa − Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科学与技术研究院）
We study Frenkel exciton-polariton Bose-Einstein condensation in a two-dimensional defect-free triangular photonic crystal with an organic semiconductor active medium containing bound excitons with dipole moments oriented perpendicular to the layers. We find photonic Bloch modes of the structure and consider their strong coupling regime with the excitonic component. Using the Gross- Pitaevskii equation for exciton polaritons and the Boltzmann equation for the external exciton reservoir, we demonstrate the formation of condensate at the points in reciprocal space where photon group velocity equ…
The similarities and differences between polariton condensation in microcavities and standard lasing in a semiconductor cavity structure are reviewed. The recent experiments on "photon condensation" are also reviewed.
Room-temperature polariton condensate in a two-dimensional hybrid perovskite
Carl von Ossietzky Universität Oldenburg（奥格斯堡卡尔冯奥西茨基大学）；University of Valencia（瓦伦西亚大学）；University of Exeter（埃克塞特大学）；Fraunhofer-Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所IOF）；Friedrich Schiller University（弗里德里希·席勒大学）；Bar-Ilan Univ.（巴伊兰大学）；Weizmann Institute of Science（魏茨曼科学研究所）
Exciton-polaritons are mixed light-matter excitations that result from the strong coupling regime between an active excitonic material and photonic resonances. Harnessing these hybrid excitations provides a rich playground to explore fascinating fundamental features, such as out-of-equilibrium Bose-Einstein condensation and quantum fluids of light, as well as novel mechanisms to be exploited in optoelectronic devices. Here, we investigate experimentally the formation of exciton-polaritons arising from the mixing between hybrid inorganic-organic perovskite excitons and an optical Bound state In…
Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both refl…
Topological physics and in particular its connection with artificial gauge fields is a forefront topic in different physical systems, ranging from cold atoms to photonics and more recently semiconductor dressed exciton-photon states, called polaritons. Engineering the energy dispersion of polaritons in microcavities through nanofabrication or exploiting the intrinsic material and cavity anisotropies has demonstrated many intriguing effects related to topology and emergent gauge fields. Here, we show that we can control the Berry curvature distribution of polariton bands in a strongly coupled o…
Achieving electrical injection of exciton-polaritons, half-light, half-matter quasiparticles arising from the strong coupling between photonic and excitonic resonances, is a crucial milestone to scale up polaritonic devices such as optical computers, quantum simulators and inversionless lasers. Here we present a new approach to achieve strong coupling between electrically injected excitons and photonic bound states in the continuum of a dielectric metasurface monolithically patterned in the channel of a light-emitting transistor. Exciton-polaritons are generated by coupling electrically inject…
Controlled Switching of Bose-Einstein Condensation in a Mixture of Two Species of Polaritons
Joint Quantum Institute, University of Maryland（马里兰大学联合量子研究所）；Department of Physics, University of Pittsburgh（匹兹堡大学物理系）；Department of Electrical Engineering, Princeton University（普林斯顿大学电气工程系）
Modulational instabilities play a key role in a wide range of nonlinear optical phenomena, leading e.g. to the formation of spatial and temporal solitons, rogue waves and chaotic dynamics. Here we experimentally demonstrate the existence of a modulational instability in condensates of cavity polaritons, arising from the strong coupling of cavity photons with quantum well excitons. For this purpose we investigate the spatiotemporal coherence properties of polariton condensates in GaAs-based microcavities under continuous-wave pumping. The chaotic behavior of the instability results in a strongl…
Excitons, bound electron-hole pairs, in Two-Dimensional Hybrid Organic Inorganic Perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E-Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E-Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E-Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstra…
Exciton-polaritons are hybrid light-matter states that arise from strong coupling between an exciton resonance and a photonic cavity mode. As bosonic excitations, they can undergo a phase transition to a condensed state that can emit coherent light without a population inversion. This aspect makes them good candidates for thresholdless lasers, yet short exciton-polariton lifetime has made it difficult to achieve condensation at very low power densities. In this sense, long-lived symmetry-protected states are excellent candidates to overcome the limitations that arise from the finite mirror ref…
For dipole-carrying excitations observed in a high-quality resonator, strong-coupling modes can appear as composite bosons with the spontaneous formation of quantized vortices in the condensed phase of a polariton fluid. In exciton-polaritons, in particular, it leads to sustained trapping of the emitted photon. In this paper, we show that magnon-polaritons can be realized due to magnon condensation caused by magnetic dipole-dipole interaction. In a quasi-2D ferrite disk placed in a microwave cavity, one observes quantum confinement effects of magnetic-dipolar-mode (MDM) oscillations. These mod…
Lead-halide perovskites are highly promising for various optoelectronic applications including laser devices. However, fundamental photophysics describing the lasing behaviour in this material family have not been investigated systematically, and thus the detailed lasing mechanism remains veiled. Here, we demonstrate that an all-inorganic perovskite shows a lasing emission based on a novel principle. A series of photoluminescence experiment results reveals that the excited state of CsPbBr3 single crystal exhibits free carrier nature. In a form of microcavity, on the other hand, the CsPbBr3 sin…
We present indications of thermalization and cooling of quasi-particles, a precursor for quantum condensation, in a plasmonic nanoparticle array. We investigate a periodic array of metallic nanorods covered by a polymer layer doped with an organic dye at room temperature. Surface lattice resonances of the array---hybridized plasmonic/photonic modes---couple strongly to excitons in the dye, and bosonic quasi-particles which we call plasmon-exciton-polaritons (PEPs) are formed. By increasing the PEP density through optical pumping, we observe thermalization and cooling of the strongly coupled PE…
Atomically thin transition metal dichalcogenides possess valley dependent functionalities that are usually available only at crogenic temperatures, constrained by various valley depolarization scatterings. The formation of exciton polaritons by coherently superimposing excitons and microcavity photons potentially harnesses the valley polarized polariton polariton interactions for novel valleytronics devices. Robust EPs have been demonstrated at room temperature in TMDs microcavity, however, the coherent polariton lasing and condensation remain elusive. Herein, we demonstrate for the first time…
Semiconductor-microcavity polaritons are composite quasiparticles of excitons and photons, emerging in the strong coupling regime. As quantum superpositions of matter and light, polaritons have much stronger interparticle interactions compared with photons, enabling rapid equilibration and Bose-Einstein condensation (BEC). Current realizations based on 1D photonic structures, such as Fabry-Pérot microcavities, have limited light-trapping ability resulting in picosecond polariton lifetime. We demonstrate, theoretically, above-room-temperature (up to 590 K) BEC of long-lived polaritons in MoSe$_…
