All-inorganic metal halides perovskites (CsPbX3, X = Br or Cl) show strong excitonic and spin-orbital coupling effects, underpinning spin-selective excitonic transitions and therefore exhibiting great promise for spintronics and quantum-optics applications. Here we report spin-dependent optical nonlinearities in CsPbX3 single crystals by using ultrafast pump-probe spectroscopy. Many-body interactions between spin-polarized excitons act like a pseudo-magnetic field and thus lift the degeneracy of spin states resulting in a photoinduced circular dichroism. Such spontaneous spin splitting between “spin-up” and “spin-down” excitons can be several tens of milli-electron volts under intense excitations. The exciton spin relaxation time is ~20 picoseconds at very low pump fluence, the longest reported in the metal halides perovskites family at room temperature. The dominant spin-flip mechanism is attributed to the electron-hole exchange interactions. Our results provide essential understandings towards realizing practical spintronics applications of perovskite semiconductors.

The quest for realizing novel fundamental physical effects and practical applications in ambient conditions has led to tremendous interest in microcavity exciton polaritons working in the strong coupling regime at room temperature. In the past few decades, a wide range of novel semiconductor systems supporting robust exciton polaritons have emerged, which has led to the realization of various fascinating phenomena and practical applications. This paper aims to review recent theoretical and experimental developments of exciton polaritons operating at room temperature, and includes a comprehensive theoretical background, descriptions of intriguing phenomena observed in various physical systems, as well as accounts of optoelectronic applications. Specifically, an in-depth review of physical systems achieving room temperature exciton polaritons will be presented, including the early development of ZnO and GaN microcavities and other emerging systems such as organics, halide perovskite semiconductors, carbon nanotubes, and transition metal dichalcogenides. Finally, a perspective of outlooking future developments will be elaborated.

Comparing with pure photons, higher nonlinearity in polariton systems has been exploited in various proof-of-principle demonstrations of efficient optical devices based on the parametric scattering effect. However, most of them demand cryogenic temperatures limited by the small exciton binding energy of traditional semiconductors or exhibit weak nonlinearity resulting from Frenkel excitons. Lead halide perovskites, possessing both a large binding energy and a strong polariton interaction, emerge as ideal platforms to explore nonlinear polariton physics toward room temperature operation. Here, we report the first observation of nonlinear parametric scattering in a lead halide perovskite microcavity with multiple polariton branches at room temperature. Driven by the scattering source from condensation in one polariton branch, correlated polariton pairs are obtained at high k states in an adjacent branch. Our results strongly advocate the ability to reach the nonlinear regime essential for perovskite polaritonics working at room temperature.

Exciton-polariton condensation is regarded as a spontaneous macroscopic quantum phenomenon with phase ordering and collective coherence. By engineering artificial annular potential landscapes in halide perovskite semiconductor microcavities, we experimentally and theoretically demonstrate the room-temperature spontaneous formation of a coherent superposition of exciton-polariton orbital states with symmetric petal-shaped patterns in real space, resulting from symmetry breaking due to the anisotropic effective potential of the birefringent perovskite crystals. The lobe numbers of such petal-shaped polariton condensates can be precisely controlled by tuning the annular potential geometry. These petal-shaped condensates form in multiple orbital states, carrying locked alternating π phase shifts and vortex–antivortex superposition cores, arising from the coupling of counterrotating exciton-polaritons in the confined circular waveguide. Our geometrically patterned microcavity exhibits promise for realizing room-temperature topological polaritonic devices and optical polaritonic switches based on periodic annular potentials.

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