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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.
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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.
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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.
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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.
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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.
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The rapid development of artificial neural networks and applied artificial intelligence has led to many applications. However, current software implementation of neural networks is severely limited in terms of performance and energy efficiency. It is believed that further progress requires the development of neuromorphic systems, in which hardware directly mimics the neuronal network structure of a human brain. Here, we propose theoretically and realize experimentally an optical network of nodes performing binary operations. The nonlinearity required for efficient computation is provided by semiconductor microcavities in the strong quantum light-matter coupling regime, which exhibit exciton-polariton interactions. We demonstrate the system performance against a pattern recognition task, obtaining accuracy on a par with state-of-the-art hardware implementations. Our work opens the way to ultrafast and energy-efficient neuromorphic systems taking advantage of ultrastrong optical nonlinearity of polaritons.
Assuntos
Inteligência Artificial , Redes Neurais de Computação , Encéfalo , Humanos , Neurônios , SemicondutoresRESUMO
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.
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Machine learning software applications are ubiquitous in many fields of science and society for their outstanding capability to solve computationally vast problems like the recognition of patterns and regularities in big data sets. In spite of these impressive achievements, such processors are still based on the so-called von Neumann architecture, which is a bottleneck for faster and power-efficient neuromorphic computation. Therefore, one of the main goals of research is to conceive physical realizations of artificial neural networks capable of performing fully parallel and ultrafast operations. Here we show that lattices of exciton-polariton condensates accomplish neuromorphic computing with outstanding accuracy thanks to their high optical nonlinearity. We demonstrate that our neural network significantly increases the recognition efficiency compared with 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 neural network architectures.
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We introduce a dynamical blockade phenomenon occurring in a nonlinear bosonic mode induced by a combination of continuous and pulsed excitations. We find that the underlying mechanism for the blockade is general, enhancing antibunching in the strongly nonlinear regime and inducing it in the weakly nonlinear regime, without fine-tuning the system parameters. Moreover, this mechanism shows advantages over existing blockade mechanisms and is suitable for implementation in a wide variety of systems due to its simplicity and universality.
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We develop a scheme of quantum reservoir state preparation, based on a quantum neural network framework, which takes classical optical excitation as input and provides desired quantum states as output. We theoretically demonstrate the broad potential of our scheme by explicitly preparing a range of intriguing quantum states, including single-photon states, Schrödinger's cat states, and two-mode entangled states. This scheme can be used as a compact quantum state preparation device for emerging quantum technologies.
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Polariton lasing is the coherent emission arising from a macroscopic polariton condensate first proposed in 1996. Over the past two decades, polariton lasing has been demonstrated in a few inorganic and organic semiconductors in both low and room temperatures. Polariton lasing in inorganic materials significantly relies on sophisticated epitaxial growth of crystalline gain medium layers sandwiched by two distributed Bragg reflectors in which combating the built-in strain and mismatched thermal properties is nontrivial. On the other hand, organic active media usually suffer from large threshold density and weak nonlinearity due to the Frenkel exciton nature. Further development of polariton lasing toward technologically significant applications demand more accessible materials, ease of device fabrication, and broadly tunable emission at room temperature. Herein, we report the experimental realization of room-temperature polariton lasing based on an epitaxy-free all-inorganic cesium lead chloride perovskite nanoplatelet microcavity. Polariton lasing is unambiguously evidenced by a superlinear power dependence, macroscopic ground-state occupation, blueshift of the ground-state emission, narrowing of the line width and the buildup of long-range spatial coherence. Our work suggests considerable promise of lead halide perovskites toward large-area, low-cost, high-performance room-temperature polariton devices and coherent light sources extending from the ultraviolet to near-infrared range.
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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.
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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.
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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.
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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.
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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.
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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.
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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.
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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.
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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.