Exciton-polaritons In Microcavities Research Articles

Solid-state continuous time crystal in a polariton condensate with a built-in mechanical clock.

Time crystals (TCs) are many-body systems that display spontaneous breaking of time translation symmetry. We demonstrate a TC by using driven-dissipative condensates of microcavity exciton-polaritons, spontaneously formed from an incoherent particle bath. The TC phases are controlled by the power of a continuous-wave nonresonant optical drive exciting the condensate and the interaction with cavity phonons. Those phases are, for increasing power, Larmor-like precession of the condensate pseudo-spins-a signature of continuous TC; locking of the frequency of precession to self-sustained coherent phonons-stabilized TC; and doubling of TC's period by phonons-a discrete TC with continuous excitation. These results establish microcavity polaritons as a platform for the investigation of time-broken symmetry in nonhermitian systems.

Hyperspectral Imaging of Exciton Polaritons in Optical Microcavities

Hyperspectral Imaging of Exciton Polaritons in Optical Microcavities

Ultra-Confined Phonon Polaritons and Strongly Coupled Microcavity Exciton Polaritons in Monolayer MoSi2N4 and WSi2N4.

The 2D semiconductors are an ideal platform for exploration of bosonic fluids composed of coupled photons and collective excitations of atoms or excitons, primarily due to large excitonic binding energies and strong light-matter interaction. Based on first-principles calculations, it is demonstrated that the phonon polaritons formed by two infrared-active phonon modes in monolayer MoSi2N4 and WSi2N4 possess ultra-high confinement factors of around ≈105 and 103, surpassing those of conventional polaritonic thin-film materials by two orders of magnitude. It is observed that the first bright exciton possesses a substantial binding energies of 750 and 740 meV in these two monolayers, with the radiative recombination lifetimes as long as 25 and 188 ns, and the Rabi splitting of the formed cavity-exciton polaritons reaching 373 and 321 meV, respectively. The effective masses of the cavity exciton polaritons are approximately 10-5me, providing the potential for high-temperature quantum condensation. The ultra-confined and ultra-low-loss phonon polaritons, as well as strongly-coupled cavity exciton polaritons with ultra-small polaritonic effective masses in these two monolayers, offering the flexible control of light at the nanoscale, probably leading to practical applications in nanophotonics, meta-optics, and quantummaterials.

Combining three sources of optical anisotropy in a tunable open-access microcavity: From theory to experiment

Photonic spin–orbit (SO) coupling is an important physical mechanism leading to numerous interesting phenomena in the systems of microcavity photons and exciton-polaritons. We report the effect of SO coupling in a tunable open-access microcavity embedded with anisotropic active media. The SO coupling associated with the TE–TM splitting results in an emergent anisotropy, which further leads to fine energy splittings allowing clear observation of the full set of eigenstates, in sharp contrast with the isotropic situation which leads to the isotropic eigenstates of spin vortices. We show that the photonic potential can be engineered by playing with the relation between the emergent anisotropy and the cavity ellipticity. All the experimental results are well reproduced by the degenerate perturbation theory. Our results constitute a significant extension to the research field of microcavity spinoptronics, with potential applications in polarization control and optical property measurement of photonic devices and materials.

Second-Order Temporal Coherence of Polariton Lasers Based on an Atomically Thin Crystal in a Microcavity.

Bosonic condensation and lasing of exciton polaritons in microcavities is a fascinating solid-state phenomenon. It provides a versatile platform to study out-of-equilibrium many-body physics and has recently appeared at the forefront of quantum technologies. Here, we study the photon statistics via the second-order temporal correlation function of polariton lasing emerging from an optical microcavity with an embedded atomically thin MoSe_{2} crystal. Furthermore, we investigate the macroscopic polariton phase transition for varying excitation powers and temperatures. The lower-polariton exhibits photon bunching below the threshold, implying a dominant thermal distribution of the emission, while above the threshold, the second-order correlation transits towards unity, which evidences the formation of a coherent state. Our findings are in agreement with a microscopic numerical model, which explicitly includes scattering with phonons on the quantum level.

Magnetically-dressed CrSBr exciton-polaritons in ultrastrong coupling regime

Over the past few decades, exciton-polaritons have attracted substantial research interest due to their half-light-half-matter bosonic nature. Coupling exciton-polaritons with magnetic orders grants access to rich many-body phenomena, but has been limited by the availability of material systems that exhibit simultaneous exciton resonances and magnetic ordering. Here we report magnetically-dressed microcavity exciton-polaritons in the van der Waals antiferromagnetic (AFM) semiconductor CrSBr coupled to a Tamm plasmon microcavity. Using angle-resolved spectroscopy, we reveal an exceptionally high exciton-photon coupling strength, up to 169 meV, demonstrating ultrastrong coupling that persists up to room temperature. By performing temperature-dependent spectroscopy, we show the magnetic nature of the exciton-polaritons in CrSBr microcavity as the magnetic order changes from AFM to paramagnetic. By applying an out-of-plane magnetic field, we achieve effective tuning of the polariton energy while maintaining the ultrastrong exciton-photon coupling strength. We attribute this to the spin canting process that modulates the interlayer exciton interaction.

Nanophotonics of microcavity exciton–polaritons

The past 30 years have witnessed remarkable developments of microcavity exciton–polaritons, which have made a great impact on photonics and optoelectronics from fundamental physics to device applications. New materials and optical structures have been developed for novel polariton lasers for the sake of room temperature operation, flexible mode engineering, and high power efficiency. More powerful spectroscopic techniques have also promoted the understanding of polariton dynamics, coherence, nonlinearity, and topology. In this review, we start with a brief introduction to the picture of polaritons, and various polariton systems based on different microcavity structures and semiconductor materials. Then, we present several important spectroscopic techniques and numerical tools for characterizing polaritons experimentally and theoretically. Next, we address the macroscopic quantum phenomena observed in the polariton systems and review the physics and applications of polariton nonlinearity. Moreover, we highlight the new emerging fields of topological and non-Hermitian polaritons. In the end, we conclude with the future perspectives of microcavity exciton–polaritons.

Independent Tuning of Exciton and Photon Energies in an Exciton–Polariton Condensate by Proton Implantation‐Induced Interdiffusion

AbstractThe use of high energy proton implantation is demonstrated to precisely and independently shift the energies of both exciton and photon components of GaAs microcavity exciton–polaritons. The technique applies post‐growth proton implantation and annealing steps in order to create a small local interdiffusion across either the quantum well–barrier material interfaces, or between the layers of the cavity distributed Bragg reflector mirrors to induce energy shifts to the exciton or photon components, respectively. The polariton mode is tunable by an energy exceeding 10 meV with a corresponding increase (decrease) in effective mass for photon (exciton) energy shifts, while maintaining narrow‐linewidth polariton photoemission and condensation for both photonic and excitonic polaritons. This technique uniquely enables new opportunities to explore coherent polariton matter with narrow‐linewidth and heavy masses in tight‐binding, non‐Hermitian, and topological landscapes with sub‐µm feature‐sizes, while also being a simple post‐growth process.

(Invited, Digital Presentation) Macroscopically Aligned Carbon Nanotubes for Photonics, Electronics, and Thermoelectrics

The remarkable flexibility, stable chemical structure, and extraordinary thermal, electrical, and optical properties of carbon nanotubes (CNTs) are promising for a variety of applications in flexible and/or high-temperature electronics, optoelectronics, and thermoelectrics, including wearables, refractory photonics, and waste heat harvesting [1]. However, the long-standing goal in the preparation of CNT ensembles is how to maintain the extraordinary properties of individual CNTs on a macroscopic scale. The polydispersity and randomness remain two main challenges.Here, we will discuss different methods for creating macroscopically aligned CNTs, including spontaneous formation of wafer-scale aligned CNT films via controlled vacuum filtration [2-4] and production of ultrahigh-conductivity CNT fibers and films through solution spinning and coating [5,6]. We will then describe the optical [2,7-11], dc and ac electrical [2,12-17], thermal [18], and thermoelectric [19-21] properties of these materials. These results are promising for device applications in various fields such as flexible CNT broadband detectors [22-26], spectrally selective thermal emitters [11], and thermoelectric devices [20,21]. W. Gao et al., “Macroscopically Aligned Carbon Nanotubes for Flexible and High-Temperature Electronics, Optoelectronics, and Thermoelectrics,” Journal of Physics D: Applied Physics 53, 063001 (2020).X. He et al., “Wafer-Scale Monodomain Films of Spontaneously Aligned Single-Walled Carbon Nanotubes,” Nature Nanotechnology 11, 633 (2016).W. Gao and J. Kono, “Science and Applications of Wafer-Scale Crystalline Carbon Nanotube Films Prepared through Controlled Vacuum Filtration,” Royal Society Open Science 6, 181605 (2019).N. Komatsu et al., “Groove-Assisted Global Spontaneous Alignment of Carbon Nanotubes in Vacuum Filtration,” Nano Letters 20, 2332 (2020).N. Behabtu et al., “Strong, Light, Multifunctional Fibers of Carbon Nanotubes with Ultrahigh Conductivity,” Science 339, 182 (2013).L. W. Taylor et al., “Improved Properties, Increased Production, and the Path to Broad Adoption of Carbon Nanotube Fibers,” Carbon 171, 689 (2021).K. Yanagi et al., “Intersubband Plasmons in the Quantum Limit in Gated and Aligned Carbon Nanotubes,” Nature Communications 9, 1121 (2018).W. Gao et al., “Continuous Transition between Weak and Ultrastrong Coupling through Exceptional Points in Carbon Nanotube Microcavity Exciton–Polaritons,” Nature Photonics 12, 362 (2018).M. E. Green et al., “Bright and Ultrafast Photoelectron Emission from Aligned Single-Wall Carbon Nanotubes through Multiphoton Exciton Resonance,” Nano Letters 19, 158 (2019).F. Katsutani et al., “Direct Observation of Cross-Polarized Excitons in Aligned Single-Chirality Single-Wall Carbon Nanotubes,” Physical Review B 99, 035426 (2019).W. Gao et al., “Macroscopically Aligned Carbon Nanotubes as a Refractory Platform for Hyperbolic Thermal Emitters,” ACS Photonics 6, 1602 (2019).X. Wang et al., “High-Ampacity Power Cables of Tightly-Packed and Aligned Carbon Nanotubes,” Advanced Functional Materials 24, 3241 (2014).A. Zubair et al., “Carbon Nanotube Fiber Terahertz Polarizer,” Applied Physics Letters 108, 141107 (2016).D. Tristant et al., “Enlightening the Ultrahigh Electrical Conductivities of Doped Double-Wall Carbon Nanotube Fibers by Raman Spectroscopy and First-Principles Calculations,” Nanoscale 18, 19668 (2016).N. Komatsu et al., “Modulation-Doped Multiple Quantum Wells of Aligned Single-Wall Carbon Nanotubes,” Advanced Functional Materials 27, 1606022 (2017).F. R. G. Bagsican et al., “Terahertz Excitonics in Carbon Nanotubes: Exciton Autoionization and Multiplication,” Nano Letters 20, 3098 (2020).A. Baydin et al., “Giant Terahertz Polarization Rotation in Ultrathin Films of Aligned Carbon Nanotubes,” Optica 8, 760 (2021).S. Yamaguchi et al., “One-Directional Thermal Transport in Densely Aligned Single-Wall Carbon Nanotube Films,” Applied Physics Letters 115, 223104 (2019).K. Fukuhara et al., “Isotropic Seebeck Coefficient of Aligned Single-Wall Carbon Nanotube Films,” Applied Physics Letters 113, 243105 (2018).Y. Ichinose et al., “Solving the Thermoelectric Trade-Off Problem with Metallic Carbon Nanotubes,” Nano Letters 19, 7370 (2019).N. Komatsu et al., “Macroscopic Weavable Fibers of Carbon Nanotubes with Giant Thermoelectric Power Factor,” Nature Communications 12, 4931 (2021).S. Nanot et al., “Broadband, Polarization-Sensitive Photodetector Based on Optically-Thick Films of Macroscopically Long, Dense, and Aligned Carbon Nanotubes,” Scientific Reports 3, 1335 (2013).X. He et al., “Photothermoelectric p-n Junction Photodetector with Intrinsic Broadband Polarimetry Based on Macroscopic Carbon Nanotube Films,” ACS Nano 7, 7271 (2013).X. He et al., “Carbon Nanotube Terahertz Detector,” Nano Letters 14, 3953 (2014).X. He, F. Léonard, and J. Kono, “Uncooled Carbon Nanotube Photodetectors,” Advanced Optical Materials 3, 989 (2015).A. Zubair et al., “Carbon Nanotube Woven Textile Photodetector,” Physical Review Materials 2, 015201 (2018).

Electrically Pumped Polarized Exciton-Polaritons in a Halide Perovskite Microcavity.

Recently, exciton-polaritons in lead halide perovskite microcavities have been extensively investigated to address striking phenomena such as polariton condensation and quantum emulation. However, a critical step in advancing these findings into practical applications, i.e., realizing electrically pumped perovskite polariton light-emitting devices, has not yet been presented. Here, we devise a new method to combine the device with a microcavity and report the first halide perovskite polariton light-emitting device. Specifically, the device is based on a CsPbBr3 capacitive structure, which can inject the electrons and holes from the same electrode, conducive to the formation of excitons and simultaneously maintaining the high quality of the microcavity. In addition, highly polarized polariton emissions have been demonstrated due to the optical birefringence in the CsPbBr3 microplate. This work paves the way for realizing practical polaritonic devices such as high-speed light-emitting devices for information communications and inversionless electrically pumped lasers based on perovskites.

Topologically driven Rabi-oscillating interference dislocation

Abstract Quantum vortices are the quantized version of classical vortices. Their center is a phase singularity or vortex core around which the flow of particles as a whole circulates and is typical in superfluids, condensates and optical fields. However, the exploration of the motion of the phase singularities in coherently-coupled systems is still underway. We theoretically analyze the propagation of an interference dislocation in the regime of strong coupling between light and matter, with strong mass imbalance, corresponding to the case of microcavity exciton–polaritons. To this end, we utilize combinations of vortex and tightly focused Gaussian beams, which are introduced through resonant pulsed pumping. We show that a dislocation originates from self-interference fringes, due to the non-parabolic dispersion of polaritons combined with moving Rabi-oscillating vortices. The morphology of singularities is analyzed in the Poincaré space for the pseudospin associated to the polariton states. The resulting beam carries orbital angular momentum with decaying oscillations due to the loss of spatial overlap between the normal modes of the polariton system.

Formation of matter-wave polaritons in an optical lattice

The polariton, a quasiparticle formed by strong coupling of a photon to a matter excitation, is a fundamental ingredient of emergent photonic quantum systems ranging from semiconductor nanophotonics to circuit quantum electrodynamics. Exploiting the interaction between polaritons has led to the realization of superfluids of light as well as of strongly correlated phases in the microwave domain, with similar efforts underway for microcavity exciton-polaritons. Here, we develop an ultracold-atom analogue of an exciton-polariton system in which interacting polaritonic phases can be studied with full tunability and without dissipation. In our optical-lattice system, the exciton is replaced by an atomic excitation, while an atomic matter wave is substituted for the photon under a strong dynamical coupling. We access the band structure of the matter-wave polariton spectroscopically by coupling the upper and lower polariton branches, and explore polaritonic many-body transport in the superfluid and Mott-insulating regimes, finding quantitative agreement with our theoretical expectations. Our work opens up novel possibilities for studies of polaritonic quantum matter.

Thermalization of Fluorescent Protein Exciton-Polaritons at Room Temperature.

Fluorescent proteins (FPs) have recently emerged as a serious contender for realizing ultralow threshold room temperature exciton-polariton condensation and lasing. This contribution investigates the thermalization of FP microcavity exciton-polaritons upon optical pumping under ambient conditions. Polariton cooling is realized using a new FP molecule, called mScarlet, coupled strongly to the optical modes in a Fabry-Pérot cavity. Interestingly, at the threshold excitation energy (fluence) of ≈9 nJ per pulse (15.6 mJ cm-2 ), an effective temperature is observed, Teff ≈ 350 ± 35 K close to the lattice temperature indicative of strongly thermalized exciton-polaritons at equilibrium. This efficient thermalization results from the interplay of radiative pumping facilitated by the energetics of the lower polariton branch and the cavity Q-factor. Direct evidence for dramatic switching from an equilibrium state into a metastable state is observed for the organic cavity polariton device at room temperature via deviation from the Maxwell-Boltzmann statistics at k‖ = 0 above the threshold. Thermalized polariton gases in organic systems at equilibrium hold substantial promise for designing room temperature polaritonic circuits, switches, and lattices for analog simulation.

Hybridized Exciton-Photon-Phonon States in a Transition Metal Dichalcogenide van der Waals Heterostructure Microcavity

Excitons in atomically thin transition-metal dichalcogenides (TMDs) have been established as an attractive platform to explore polaritonic physics, owing to their enormous binding energies and giant oscillator strength. Basic spectral features of exciton polaritons in TMD microcavities, thus far, were conventionally explained via two-coupled-oscillator models. This ignores, however, the impact of phonons on the polariton energy structure. Here we establish and quantify the threefold coupling between excitons, cavity photons, and phonons. For this purpose, we employ energy-momentum-resolved photoluminescence and spatially resolved coherent two-dimensional spectroscopy to investigate the spectral properties of a high-quality-factor microcavity with an embedded WSe_{2} van der Waals heterostructure at room temperature. Our approach reveals a rich multibranch structure which thus far has not been captured in previous experiments. Simulation of the data reveals hybridized exciton-photon-phonon states, providing new physical insight into the exciton polariton system based on layered TMDs.

Phase Transitions of Exciton-Polaritons in Grating-Based Microcavities

Phase Transitions of Exciton-Polaritons in Grating-Based Microcavities

Microcavity exciton polaritons at room temperature

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.

Exciton-polariton properties of hexagonal BN-based microcavity and their potential applications in BEC and superconductivity

Microcavity exciton-polaritons are two-dimensional bosonic quasiparticles composed by excitons and photons. Using a model Hamiltonian with parameters generated from ab initio density-functional theory and Bethe-Salpeter equation calculations, we investigate the exciton and the exciton-polariton properties of hexagnonal boron nitride (hBN) based microcavity. We show that hBN-based microcavities, including monolayer and all-dielectric ones, are promising in optoelectronic applications. Room temperature exciton-polariton Bose-Einstein condensation can be achieved because of the large oscillator strength and binding energy of the exciton, and the strong interaction between the exciton-polaritons and the longitudinal optical phonons. Based on this BEC state, an exciton-polariton mediated superconducting device can also be fabricated at a few tens of kelvin using the microcavity structure proposed by Laussy et al. Phys. Rev. Lett. 104, 106402 (2010).

Collective Excitations of Exciton-Polariton Condensates in a Synthetic Gauge Field.

Collective (elementary) excitations of quantum bosonic condensates, including condensates of exciton polaritons in semiconductor microcavities, are a sensitive probe of interparticle interactions. In anisotropic microcavities with momentum-dependent transverse-electric-transverse-magnetic splitting of the optical modes, the excitations' dispersions are predicted to be strongly anisotropic, which is a consequence of the synthetic magnetic gauge field of the cavity, as well as the interplay between different interaction strengths for polaritons in the singlet and triplet spin configurations. Here, by directly measuring the dispersion of the collective excitations in a high-density optically trapped exciton-polariton condensate, we observe excellent agreement with the theoretical predictions for spinor polariton excitations. We extract the interaction constants for polaritons of the same and opposite spin and map out the characteristic spin textures in an interacting spinor condensate of exciton polaritons.

Erratum: Microscopic description of exciton-polaritons in microcavities [Phys. Rev. Research 1 , 033120 (2019)

Erratum: Microscopic description of exciton-polaritons in microcavities [Phys. Rev. Research 1 , 033120 (2019)

Finite-temperature Hartree-Fock-Bogoliubov theory for exciton-polaritons

Microcavity exciton-polaritons, known to exhibit nonequilibrium Bose condensation at high critical temperatures, can also be brought in thermal equilibrium with the surrounding medium and form a quantum degenerate Bose-Einstein distribution. It happens when their thermalization time in the regime of positive detunings---or, alternatively, for high-finesse microcavities---becomes shorter than their lifetime. Here we present the self-consistent finite-temperature Hartree--Fock--Bogoliubov description for such a system of polaritons, universally addressing the excitation spectrum, momentum-dependent interactions, condensate depletion, and the background population of dark excitons that contribute to the system's chemical potential. Employing the derived expressions, we discuss the implications for the Bogoliubov sound velocity, confirmed by existing experiments, and define the critical temperatures of (quasi)condensation and the integral particle lifetime dependencies on the detuning. Large positive detunings are shown to provide conditions for the total lifetime reaching nanosecond timescales. This allows realization of thermodynamically equilibrium polariton systems with Bose-Einstein condensate forming at temperatures as high as tens of Kelvin.