Trembling Motion of Exciton Polaritons Close to the Rashba-Dresselhaus Regime.

We report the experimental observation of trembling quantum motion, or Zitterbewegung, of exciton polaritons in a perovskite microcavity at room temperature. By introducing liquid-crystal molecules into the microcavity, we achieve spinor states with synthetic Rashba-Dresselhaus spin-orbit coupling and tunable energy splitting. Under a resonant excitation, the polariton fluid exhibits clear trembling motion perpendicular to its flowing direction, accompanied by a unique spin pattern resembling interlocked fingers. Furthermore, leveraging the sizable tunability of energy gaps by external electrical voltages, we observe the continuous transition of polariton Zitterbewegung from relativistic (small gaps) to nonrelativistic (large gaps) regimes. Our findings pave the way for using exciton polaritons in the emulation of relativistic quantum physics.

Strong light-matter coupling in van der Waals materials.

In recent years, two-dimensional (2D) van der Waals materials have emerged as a focal point in materials research, drawing increasing attention due to their potential for isolating and synergistically combining diverse atomic layers. Atomically thin transition metal dichalcogenides (TMDs) are one of the most alluring van der Waals materials owing to their exceptional electronic and optical properties. The tightly bound excitons with giant oscillator strength render TMDs an ideal platform to investigate strong light-matter coupling when they are integrated with optical cavities, providing a wide range of possibilities for exploring novel polaritonic physics and devices. In this review, we focused on recent advances in TMD-based strong light-matter coupling. In the foremost position, we discuss the various optical structures strongly coupled to TMD materials, such as Fabry-Perot cavities, photonic crystals, and plasmonic nanocavities. We then present several intriguing properties and relevant device applications of TMD polaritons. In the end, we delineate promising future directions for the study of strong light-matter coupling in van der Waals materials.

Room temperature polariton spin switches based on Van der Waals superlattices.

Transition-metal dichalcogenide monolayers possess large exciton binding energy and a robust valley degree of freedom, making them a viable platform for the development of spintronic devices capable of operating at room temperature. The development of such monolayer TMD-based spintronic devices requires strong spin-dependent interactions and effective spin transport. This can be achieved by employing exciton-polaritons. These hybrid light-matter states arising from the strong coupling of excitons and photons allow high-speed in-plane propagation and strong nonlinear interactions. Here, we demonstrate the operation of all-optical polariton spin switches by incorporating a WS2 superlattice into a planar microcavity. We demonstrate spin-anisotropic polariton nonlinear interactions in a WS2 superlattice at room temperature. As a proof-of-concept, we utilize these spin-dependent interactions to implement different spin switch geometries at ambient conditions, which show intrinsic sub-picosecond switching time and small footprint. Our findings offer new perspectives on manipulations of the polarization state in polaritonic systems and highlight the potential of atomically thin semiconductors for the development of next generation information processing devices.

Spatial Filtering of Interlayer Exciton Ground State in WSe2/MoS2 Heterobilayer.

Long-life interlayer excitons (IXs) in transition metal dichalcogenide (TMD) heterostructure are promising for realizing excitonic condensates at high temperatures. Critical to this objective is to separate the IX ground state (the lowest energy of IX state) emission from other states' emissions. Filtering the IX ground state is also essential in uncovering the dynamics of correlated excitonic states, such as the excitonic Mott insulator. Here, we show that the IX ground state in the WSe2/MoS2 heterobilayer can be separated from other states by its spatial profile. The emissions from different moiré IX modes are identified by their different energies and spatial distributions, which fits well with the rate-diffusion model for cascading emission. Our results show spatial filtering of the ground state mode and enrich the toolbox to realize correlated states at elevated temperatures.

Origin of Exciton-Polariton Interactions and Decoupled Dark States Dynamics in 2D Hybrid Perovskite Quantum Wells.

The realization of efficient optical devices depends on the ability to harness strong nonlinearities, which are challenging to achieve with standard photonic systems. Exciton-polaritons formed in hybrid organic-inorganic perovskites offer a promising alternative, exhibiting strong interactions at room temperature (RT). Despite recent demonstrations showcasing a robust nonlinear response, further progress is hindered by an incomplete understanding of the microscopic mechanisms governing polariton interactions in perovskite-based strongly coupled systems. Here, we investigate the nonlinear properties of quasi-2D dodecylammonium lead iodide perovskite (n3-C12) crystals embedded in a planar microcavity. Polarization-resolved pump-probe measurements reveal the contribution of indirect exchange interactions assisted by dark states formation. Additionally, we identify a strong dependence of the unique spin-dependent interaction of polaritons on sample detuning. The results are pivotal for the advancement of polaritonics, and the tunability of the robust spin-dependent anisotropic interaction in n3-C12 perovskites makes this material a powerful choice for the realization of polaritonic circuits.

Energy transfer driven brightening of MoS2 by ultrafast polariton relaxation in microcavity MoS2/hBN/WS2 heterostructures.

Energy transfer is a ubiquitous phenomenon that delivers energy from a blue-shifted emitter to a red-shifted absorber, facilitating wide photonic applications. Two-dimensional (2D) semiconductors provide unique opportunities for exploring novel energy transfer mechanisms in the atomic-scale limit. Herein, we have designed a planar optical microcavity-confined MoS2/hBN/WS2 heterojunction, which realizes the strong coupling among donor exciton, acceptor exciton, and cavity photon mode. This configuration demonstrates an unconventional energy transfer via polariton relaxation, brightening MoS2 with a record-high enhancement factor of ~440, i.e., two-order-of-magnitude higher than the data reported to date. The polariton relaxation features a short characteristic time of ~1.3 ps, resulting from the significantly enhanced intra- and inter-branch exciton-exciton scattering. The polariton relaxation dynamics is associated with Rabi energies in a phase diagram by combining experimental and theoretical results. This study opens a new direction of microcavity 2D semiconductor heterojunctions for high-brightness polaritonic light sources and ultrafast polariton carrier dynamics.

Controllable vortex lasing arrays in a geometrically frustrated exciton-polariton lattice at room temperature.

Quantized vortices appearing in topological excitations of quantum phase transition play a pivotal role in strongly correlated physics involving the underlying confluence of superfluids, Bose-Einstein condensates and superconductors. Exciton polaritons as bosonic quasiparticles have enabled studies of non-equilibrium quantum gases and superfluidity. Exciton-polariton condensates in artificial lattices intuitively emulate energy-band structures and quantum many-body effects of condensed matter, underpinning constructing vortex lattices and controlling quantum fluidic circuits. Here, we harness exciton-polariton quantum fluids of light in a frustrated kagome lattice based on robust metal-halide perovskite microcavities, to demonstrate vortex lasing arrays and modulate their configurations at room temperature. Tomographic energy-momentum spectra unambiguously reveal massless Dirac bands and quenched kinetic-energy flat bands coexisting in kagome lattices, where polariton condensates exhibit prototypical honeycomb and kagome spatial patterns. Spatial coherence investigations illustrate two types of phase textures of polariton condensates carrying ordered quantized-vortex arrays and π-phase shifts, which could be selected when needed using lasing emission energy. Our findings offer a promising platform on which it is possible to study quantum-fluid correlations in complex polaritonic lattices and highlight feasible applications of structured light.

Higher-order topological polariton corner state lasing.

Unlike conventional laser, the topological laser is able to emit coherent light robustly against disorders and defects because of its nontrivial band topology. As a promising platform for low-power consumption, exciton polariton topological lasers require no population inversion, a unique property that can be attributed to the part-light-part-matter bosonic nature and strong nonlinearity of exciton polaritons. Recently, the discovery of higher-order topology has shifted the paradigm of topological physics to topological states at boundaries of boundaries, such as corners. However, such topological corner states have never been realized in the exciton polariton system yet. Here, on the basis of an extended two-dimensional Su-Schrieffer-Heeger lattice model, we experimentally demonstrate the topological corner states of perovskite polaritons and achieved polariton corner state lasing with a low threshold (approximately microjoule per square centimeter) at room temperature. The realization of such polariton corner states also provides a mechanism of polariton localization under topological protection, paving the way toward on-chip active polaritonics using higher-order topology.

Exciton polariton interactions in Van der Waals superlattices at room temperature.

Monolayer transition-metal dichalcogenide (TMD) materials have attracted a great attention because of their unique properties and promising applications in integrated optoelectronic devices. Being layered materials, they can be stacked vertically to fabricate artificial van der Waals lattices, which offer unique opportunities to tailor the electronic and optical properties. The integration of TMD heterostructures in planar microcavities working in strong coupling regime is particularly important to control the light-matter interactions and form robust polaritons, highly sought for room temperature applications. Here, we demonstrate the systematic control of the coupling-strength by embedding multiple WS2 monolayers in a planar microcavity. The vacuum Rabi splitting is enhanced from 36 meV for one monolayer up to 72 meV for the four-monolayer microcavity. In addition, carrying out time-resolved pump-probe experiments at room temperature we demonstrate the nature of polariton interactions which are dominated by phase space filling effects. Furthermore, we also observe the presence of long-living dark excitations in the multiple monolayer superlattices. Our results pave the way for the realization of polaritonic devices based on planar microcavities embedding multiple monolayers and could potentially lead the way for future devices towards the exploitation of interaction-driven phenomena at room temperature.

Optically trapped room temperature polariton condensate in an organic semiconductor.

The strong nonlinearities of exciton-polariton condensates in lattices make them suitable candidates for neuromorphic computing and physical simulations of complex problems. So far, all room temperature polariton condensate lattices have been achieved by nanoimprinting microcavities, which by nature lacks the crucial tunability required for realistic reconfigurable simulators. Here, we report the observation of a quantised oscillating nonlinear quantum fluid in 1D and 2D potentials in an organic microcavity at room temperature, achieved by an on-the-fly fully tuneable optical approach. Remarkably, the condensate is delocalised from the excitation region by macroscopic distances, leading both to longer coherence and a threshold one order of magnitude lower than that with a conventional Gaussian excitation profile. We observe different mode selection behaviour compared to inorganic materials, which highlights the anomalous scaling of blueshift with pump intensity and the presence of sizeable energy-relaxation mechanisms. Our work is a major step towards a fully tuneable polariton simulator at room temperature.

Limit cycles and chaos in the hybrid atom-optomechanics system.

We consider atoms in two different periodic potentials induced by different lasers, one of which is coupled to a mechanical membrane via radiation pressure force. The atoms are intrinsically two-level systems that can absorb or emit photons, but the dynamics of their position and momentum are treated classically. On the other hand, the membrane, the cavity field, and the intrinsic two-level atoms are treated quantum mechanically. We show that the mean excitation of the three systems can be stable, periodically oscillating, or in a chaotic state depending on the strength of the coupling between them. We define regular, limit cycle, and chaotic phases, and present a phase diagram where the three phases can be achieved by manipulating the field-membrane and field-atom coupling strengths. We also computed other observable quantities that can reflect the system's phase such as position, momentum, and correlation functions. Our proposal offers a new way to generate and tune the limit cycle and chaotic phases in a well-established atom-optomechanics system.

Electric Field Modulation of 2D Perovskite Excitonics.

Multiquantum-well (MQW) perovskite is one of the forerunners in high-efficiency perovskite LED (PeLEDs) research. Despite the rapid inroads, PeLEDs suffer from the pertinent issue of efficiency decrease with increasing brightness, commonly known as "efficiency roll-off". The underlying mechanisms are presently an open question. Herein, we explicate the E-field effects on the exciton states in the archetypal MQW perovskite (C6H5C2H4NH3)2PbI4, or PEPI, in a device-like architecture using field-assisted transient spectroscopy and theoretical modeling. The applied E-field results in a complex interplay of spectral blueshifts and enhancement/quenching of the different exciton modes. The former originates from the DC Stark shift, while the latter is attributed to the E-field modulation of the transfer rates between bright/dark exciton modes. Importantly, our findings uncover crucial insights into the photophysical processes under E-field modulation contributing to efficiency roll-off in MQW PeLEDs. Electrical modulation of exciton properties presents exciting possibilities for signal processing devices.

Nonlinear polariton parametric emission in an atomically thin semiconductor based microcavity.

Parametric nonlinear optical processes are at the heart of nonlinear optics underpinning the central role in the generation of entangled photons as well as the realization of coherent optical sources. Exciton-polaritons are capable to sustain parametric scattering at extremely low threshold, offering a readily accessible platform to study bosonic fluids. Recently, two-dimensional transition-metal dichalcogenides (TMDs) have attracted great attention in strong light-matter interactions due to robust excitonic transitions and unique spin-valley degrees of freedom. However, further progress is hindered by the lack of realizations of strong nonlinear effects in TMD polaritons. Here, we demonstrate a realization of nonlinear optical parametric polaritons in a WS2 monolayer microcavity pumped at the inflection point and triggered in the ground state. We observed the formation of a phase-matched idler state and nonlinear amplification that preserves the valley population and survives up to room temperature. Our results open a new door towards the realization of the future for all-optical valley polariton nonlinear devices.

Giant Enhancement of Unconventional Photon Blockade in a Dimer Chain.

Unconventional photon blockade refers to the suppression of multiphoton states in weakly nonlinear optical resonators via the destructive interference of different excitation pathways. It has been studied in a pair of coupled nonlinear resonators and other few-mode systems. Here, we show that unconventional photon blockade can be greatly enhanced in a chain of coupled resonators. The strength of the nonlinearity in each resonator needed to achieve unconventional photon blockade is suppressed exponentially with lattice size. The analytic derivation, based on a weak drive approximation, is validated by wave function Monte Carlo simulations. These findings show that customized lattices of coupled resonators can be powerful tools for controlling multiphoton quantum states.

Direct measurement of a non-Hermitian topological invariant in a hybrid light-matter system.

Topology is central to understanding and engineering materials that display robust physical phenomena immune to imperfections. Different topological phases of matter are characterized by topological invariants. In energy-conserving (Hermitian) systems, these invariants are determined by the winding of eigenstates in momentum space. In non-Hermitian systems, a topological invariant is predicted to emerge from the winding of the complex eigenenergies. Here, we directly measure the non-Hermitian topological invariant arising from exceptional points in the momentum-resolved spectrum of exciton polaritons. These are hybrid light-matter quasiparticles formed by photons strongly coupled to electron-hole pairs (excitons) in a halide perovskite semiconductor at room temperature. We experimentally map out both the real (energy) and imaginary (linewidth) parts of the spectrum near the exceptional points and extract the novel topological invariant­fractional spectral winding. Our work represents an essential step toward realization of non-Hermitian topological phases in a condensed matter system.

All-optical switching based on interacting exciton polaritons in self-assembled perovskite microwires.

Ultrafast all-optical switches and integrated circuits call for giant optical nonlinearity to minimize energy consumption and footprint. Exciton polaritons underpin intrinsic strong nonlinear interactions and high-speed propagation in solids, thus affording an intriguing platform for all-optical devices. However, semiconductors sustaining stable exciton polaritons at room temperature usually exhibit restricted nonlinearity and/or propagation properties. Delocalized and strongly interacting Wannier-Mott excitons in metal halide perovskites highlight their advantages in integrated nonlinear optical devices. Here, we report all-optical switching by using propagating and strongly interacting exciton-polariton fluids in self-assembled CsPbBr3 microwires. Strong polariton-polariton interactions and extended polariton fluids with a propagation length of around 25 µm have been reached. All-optical switching on/off of polariton propagation can be realized in picosecond time scale by locally blue-shifting the dispersion with interacting polaritons. The all-optical switching, together with the scalable self-assembly method, highlights promising applications of solution-processed perovskites toward integrated photonics operating in strong coupling regime.

Perovskite semiconductors for room-temperature exciton-polaritonics.

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.

Optical switching of topological phase in a perovskite polariton lattice.

Strong light-matter interaction enriches topological photonics by dressing light with matter, which provides the possibility to realize active nonlinear 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. Previous demonstrations of exciton polariton topological insulators demand cryogenic temperatures, and their topological properties are usually fixed. Here, we experimentally demonstrate a room temperature exciton polariton topological insulator in a perovskite zigzag lattice. Polarization serves as a degree of freedom to switch between distinct topological phases, and the topologically nontrivial polariton edge states persist in the presence of onsite energy perturbations, showing strong immunity to disorder. We further demonstrate exciton polariton condensation into the topological edge states under optical pumping. These results provide an ideal platform for realizing active topological polaritonic devices working at ambient conditions, which can find important applications in topological lasers, optical modulation, and switching.

Ultralow Threshold Polariton Condensate in a Monolayer Semiconductor Microcavity at Room Temperature.

Exciton-polaritons, hybrid light-matter bosonic quasiparticles, can condense into a single quantum state, i.e., forming a polariton Bose-Einstein condensate (BEC), which represents a crucial step for the development of nanophotonic technology. Recently, atomically thin transition-metal dichalcogenides (TMDs) emerged as promising candidates for novel polaritonic devices. Although the formation of robust valley-polaritons has been realized up to room temperature, the demonstration of polariton lasing remains elusive. Herein, we report for the first time the realization of this important milestone in a TMD microcavity at room temperature. Continuous wave pumped polariton lasing is evidenced by the macroscopic occupation of the ground state, which undergoes a nonlinear increase of the emission along with the emergence of temporal coherence, the presence of an exciton fraction-controlled threshold and the buildup of linear polarization. Our work presents a critically important step toward exploiting nonlinear polariton-polariton interactions, as well as offering a new platform for thresholdless lasing.

Nonlinear Parametric Scattering of Exciton Polaritons in Perovskite Microcavities.

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.