The invention and development of the laser have revolutionized science, technology, and industry. Metal halide perovskites are an emerging class of semiconductors holding promising potential in further advancing the laser technology. In this Review, we provide a comprehensive overview of metal halide perovskite lasers from the viewpoint of materials chemistry and engineering. After an introduction to the materials chemistry and physics of metal halide perovskites, we present diverse optical cavities for perovskite lasers. We then comprehensively discuss various perovskite lasers with particular functionalities, including tunable lasers, multicolor lasers, continuous-wave lasers, single-mode lasers, subwavelength lasers, random lasers, polariton lasers, and laser arrays. Following this a description of the strategies for improving the stability and reducing the toxicity of metal halide perovskite lasers is provided. Finally, future research directions and challenges toward practical technology applications of perovskite lasers are provided to give an outlook on this emerging field.

Materials chemistry and engineering in metal halide perovskite lasers

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 as lattices of trapped ions and superconducting circuit arrays also rely on ultracold temperatures. Exciton polaritons with extremely light effective mass, are regarded as promising alternatives to realize Bose-Einstein condensation in lattices at higher temperatures. Along with the condensation, an efficient exciton polariton quantum simulator would require a strong lattice with robust trapping at each lattice site as well as strong inter-site coupling to allow coherent quantum motion of polaritons within the lattice. However, exciton polaritons in a strong lattice have only been shown to condense at liquid helium temperatures. Here, we report the observation of exciton polariton condensation in a one-dimensional strong lead halide perovskite lattice at room temperature. Modulated by deep periodic potentials, the strong lead halide perovskite lattice exhibits a large forbidden bandgap opening up to 13.3 meV and a lattice band up to 8.5 meV wide, which are at least 10 times larger than previous systems. Above a critical density, we observe exciton polariton condensation into py orbital states with long-range spatial coherence at room temperature. Our result opens the route to the implementation of polariton condensates in quantum simulators at room temperature.

Observation of Exciton Polariton Condensation in a Perovskite Lattice at Room Temperature

We demonstrate an organic polariton condensate that exhibits nonlinear interactions at room-temperature. Upon reaching threshold, we observe a superlinear power dependence, a power-dependent blueshift and the emergence of long-range spatial coherence resulting from polariton interactions.

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Nonlinear interactions in an organic polariton condensate

Lead-halide perovskites are generally excellent light emitters and can have larger exciton binding energies than thermal energy at room temperature, exhibiting great promise for room-temperature exciton-polaritonics. Rapid progress has been made recently, although challenges and mysteries remain in lead-halide perovskite semiconductors to push polaritons to room-temperature operation. In this Perspective, we discuss fundamental aspects of perovskite semiconductors for exciton-polaritons and review the recent rapid experimental advances using lead-halide perovskites for room-temperature polaritonics, including the experimental realization of strong light–matter interaction using various types of microcavities as well as reaching the polariton condensation regime in planar microcavities and lattices. An outlook on the potential of lead-halide perovskites as a playground for exciton-polariton studies and for the development of polaritonic devices operating at room temperature is provided.

Perovskite semiconductors for room-temperature exciton-polaritonics.

While halide perovskites (HPs) have achieved enormous success in the field of optoelectronic applications, much attention has been recently drawn to the unique polarization sensitivity of HPs, either intrinsic or extrinsic, which makes HPs a potential candidate for innovative applications in directly polarized luminescence and detection. Herein, the research status in the field of polarization-sensitive HPs, including linear polarization and circular polarization, is comprehensively summarized. To evaluate the effectiveness of HPs in generating and detecting linearly or circularly polarized light, the principles and characterization methods of polarized luminescence and detection are introduced. Sequentially, the state-of-the-art development of the strategies that induce the linear or circular polarization characteristics of HPs is systematically reviewed, based on which the application of polarization-sensitive HPs in the field of polarization luminescence and detection are summarized. Moreover, the current challenges and opportunities are discussed, and prospects of the future development in this promising field are outlined.

Polarization-Sensitive Halide Perovskites for Polarized Luminescence and Detection: Recent Advances and Perspectives.

The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid-state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principal value exhibit strong dipole-dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, we observe the formation of REPs in a single crystal CsPbBr3 perovskite cavity without any external fields. These polaritons exhibit strong nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr3 are highly anisotropic and have a large extinction ratio, arising from the perovskite's orthorhombic crystal structure. Our observation not only sheds light on the importance of many-body physics in coherent polariton systems involving higher-order excited states, but also paves the way for exploring these coherent interactions for solid-state quantum optical information processing.

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity.

The condensation of half-light half-matter exciton polaritons in semiconductor optical cavities is a striking example of macroscopic quantum coherence in a solid state platform. Quantum coherence is possible only when there are strong interactions between the exciton polaritons provided by their excitonic constituents. Rydberg excitons with high principle value exhibit strong dipole-dipole interactions in cold atoms. However, polaritons with the excitonic constituent that is an excited state, namely Rydberg exciton polaritons (REPs), have not yet been experimentally observed. Here, for the first time, we observe the formation of REPs in a single crystal CsPbBr3 perovskite cavity without any external fields. These polaritons exhibit strong nonlinear behavior that leads to a coherent polariton condensate with a prominent blue shift. Furthermore, the REPs in CsPbBr3 are highly anisotropic and have a large extinction ratio, arising from the perovskite's orthorhombic crystal structure. Our observation not only sheds light on the importance of many-body physics in coherent polariton systems involving higher-order excited states, but also paves the way for exploring these coherent interactions for solid state quantum optical information processing.

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity

Exciton polaritons, the part-light and part-matter quasiparticles in semiconductor optical cavities, are promising for exploring Bose–Einstein condensation, non-equilibrium many-body physics and analogue simulation at elevated temperatures. However, a room-temperature polaritonic platform on par with the GaAs quantum wells grown by molecular beam epitaxy at low temperatures remains elusive. The operation of such a platform calls for long-lifetime, strongly interacting excitons in a stringent material system with large yet nanoscale-thin geometry and homogeneous properties. Here, we address this challenge by adopting a method based on the solution synthesis of excitonic halide perovskites grown under nanoconfinement. Such nanoconfinement growth facilitates the synthesis of smooth and homogeneous single-crystalline large crystals enabling the demonstration of XY Hamiltonian lattices with sizes up to 10 × 10. With this demonstration, we further establish perovskites as a promising platform for room temperature polaritonic physics and pave the way for the realization of robust mode-disorder-free polaritonic devices at room temperature. The realization of large-scale exciton–polariton platforms operating at room temperature and exhibiting long-lived, strongly interacting excitons has been elusive. Here, the authors demonstrate a room-temperature perovskite-based polaritonic platform with a polariton lattice size of up to 10 × 10. 

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Halide perovskites enable polaritonic XY spin Hamiltonian at room temperature

Abstract Quantum fluids exhibit quantum mechanical effects at the macroscopic level, which contrast strongly with classical fluids. Gain-dissipative solid-state exciton-polaritons systems are promising emulation platforms for complex quantum fluid studies at elevated temperatures. Recently, halide perovskite polariton systems have emerged as materials with distinctive advantages over other room-temperature systems for future studies of topological physics, non-Abelian gauge fields, and spin-orbit interactions. However, the demonstration of nonlinear quantum hydrodynamics, such as superfluidity and Čerenkov flow, which is a consequence of the renormalized elementary excitation spectrum, remains elusive in halide perovskites. Here, using homogenous halide perovskites single crystals, we report, in both one- and two-dimensional cases, the complete set of quantum fluid phase transitions from normal classical fluids to scatterless polariton superfluids and supersonic fluids—all at room temperature, clear consequences of the Landau criterion. Specifically, the supersonic Čerenkov wave pattern was observed at room temperature. The experimental results are also in quantitative agreement with theoretical predictions from the dissipative Gross-Pitaevskii equation. Our results set the stage for exploring the rich non-equilibrium quantum fluid many-body physics at room temperature and also pave the way for important polaritonic device applications. 

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Renjie Tao

Papers

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity.

Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity

Halide perovskites enable polaritonic XY spin Hamiltonian at room temperature

Room-temperature polariton quantum fluids in halide perovskites