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Exciton polaritons in atomically thin transition metal dichalcogenide crystals (monolayer TMDCs) have emerged as a promising candidate to enable topological transport, ultra-efficient laser technologies, and collective quantum phenomena such as polariton condensation and superfluidity at room temperature. However, integrating monolayer TMDCs into high-quality planar microcavities to achieve the required strong coupling between the cavity photons and the TMDC excitons (bound electron–hole pairs) has proven challenging. Previous approaches to integration had to compromise between various adverse effects on the strength of light–matter interactions in the monolayer, the cavity photon lifetime, and the lateral size of the microcavity. Here, we demonstrate a scalable approach to fabricate high-quality planar microcavities with an integrated monolayer WS2 layer-by-layer by using polymethyl methacrylate/silicon oxide (PMMA/SiO x) as a cavity spacer. Because the exciton oscillator strength is well protected against the required processing steps by the PMMA layer, the microcavities investigated in this work, which have quality factors of above 103, can operate in the strong light–matter coupling regime at room temperature. This is an important step toward fabricating wafer-scale and patterned microcavities for engineering the exciton-polariton potential landscape, which is essential for enabling many proposed technologies.

We investigate the effects of direct deposition of different dielectric materials (AlOx, SiOx, SiNx) onto atomically thin TMDC WS2 on its optical response using atomic layer deposition (ALD), electron beam evaporation (EBE), plasma-enhanced chemical vapor deposition (PECVD), and magnetron sputtering. The photoluminescence measurements reveal quenching of the excitonic emission after all deposition processes, which is linked to the increased level of charge doping and associated rise of the trion emission and/or the localized (bound) exciton emission. Furthermore, Raman spectroscopy allows us to clearly correlate the observed changes in excitonic emission with the increased levels of lattice disorder and defects. In particular, we show that the different doping levels in a monolayer WS2 capped by a dielectric material are strongly related to the defects in the WS2 crystal introduced by all capping methods, except for ALD. The strong charge doping in the ALD-capped sample seems to be caused by other factors, such as deviations in the dielectric layer stoichiometry or chemical reactions on the monolayer surface, which makes ALD distinct from all other techniques. Overall, the EBE process results in the lowest level of doping and defect densities and in the largest spectral weight of the exciton emission in the PL. Sputtering is revealed as the most aggressive dielectric capping method for WS2, fully quenching its optical response. Our results demonstrate and quantify the effects of direct deposition of dielectric materials onto monolayer WS2, which can provide valuable guidance for the efforts to integrate monolayer TMDCs into functional optoelectronic devices.

Topological insulators are a class of electronic materials exhibiting robust edge states immune to perturbations and disorder. This concept has been successfully adapted in photonics, where topologically nontrivial waveguides and topological laserswere developed.However, the exploration of topological properties in a given photonic system is limited to a fabricated sample, without the flexibility to reconfigure the structure in situ.Here, we demonstrate an all-optical realization of the orbital Su-Schrieffer-Heeger model in a microcavity exciton-polariton system, whereby a cavity photon is hybridized with an exciton in a GaAs quantum well.We induce a zigzag potential for exciton polaritons all-optically by shaping the nonresonant laser excitation, and measure directly the eigenspectrum and topological edge states of a polariton lattice in a nonlinear regime of bosonic condensation. Furthermore, taking advantage of the tunability of the optically induced lattice, we modify the intersite tunneling to realize a topological phase transition to a trivial state.Our results open the way to study topological phase transitions on-demand in fully reconfigurable hybrid photonic systems that do not require sophisticated sample engineering. Ministry of Education (MOE) Published version Australian Research Council (CE170100039); Ministry of Education–Singapore (MOE2018-T3-1-002, MOE2019-T2-1-004); Narodowe Centrum Nauki (2018/30/E/ST7/00648); Fundacja na rzecz Nauki Polskiej (START); National Science Foundation (DMR-2004570).

Description, A non-Hermitian topological invariant arising from exceptional points is directly probed in an exciton-polariton 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 invariant—fractional spectral winding. Our work represents an essential step toward realization of non-Hermitian topological phases in a condensed matter system.

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.

Monolayer transition metal dichalcogenides are a promising platform to investigate many-body interactions of excitonic complexes. In monolayer tungsten diselenide, the ground-state exciton is dark (spin-indirect), and the valley degeneracy allows low-energy dark momentum-indirect excitons to form. Interactions between the dark exciton species and the optically accessible bright exciton (X) are likely to play significant roles in determining the optical properties of X at high power, as well as limiting the ultimate exciton densities that can be achieved, yet so far little is known about these interactions. Here, we demonstrate long-lived dense populations of momentum-indirect intervalley ($X_K$) and spin-indirect intravalley (D) dark excitons by time-resolved photoluminescence measurements (Tr-PL). Our results uncover an efficient inter-state conversion between X to D excitons through the spin-flip process and the one between D and $X_K$ excitons mediated by the exchange interaction (D + D to $X_K$ + $X_K$). Moreover, we observe a persistent redshift of the X exciton due to strong excitonic screening by $X_K$ exciton with a response time in the timescale of sub-ns, revealing a non-trivial inter-state exciton-exciton interaction. Our results provide a new insight into the interaction between bright and dark excitons, and point to a possibility to employ dark excitons for investigating exciton condensation and the valleytronics.

Atomically thin transition metal dichalcogenide crystals (TMDCs) have extraordinary optical properties that make them attractive for future optoelectronic applications. Integration of TMDCs into practical all-dielectric heterostructures hinges on the ability to passivate and protect them against necessary fabrication steps on large scales. Despite its limited scalability, encapsulation of TMDCs in hexagonal boron nitride (hBN) currently has no viable alternative for achieving high performance of the final device. Here, it is shown that the novel, ultrathin Ga

We report the observation of low-energy, low-momenta collective oscillations of an excitonpolariton condensate in a round "box" trap. The oscillations are dominated by the dipole and breathing modes, and the ratio of the frequencies of the two modes is consistent with that of a weakly interacting two-dimensional trapped Bose gas. The speed of sound extracted from the dipole oscillation frequency is smaller than the Bogoliubov sound, which can be partly explained by the influence of the incoherent reservoir. These results pave the way for understanding the effects of reservoir, dissipation, energy relaxation, and finite temperature on the superfluid properties of exciton-polariton condensates and other two-dimensional open-dissipative quantum fluids., Comment: 13 pages, 15 figures

Exciton-polaritons (polaritons herein) offer a unique nonlinear platform for studies of collective macroscopic quantum phenomena in a solid state system. Shaping of polariton flow and polariton confinement via potential landscapes created by nonresonant optical pumping has gained considerable attention due to the degree of flexibility and control offered by optically-induced potentials. Recently, large density-dependent energy shifts (blueshifts) exhibited by optically trapped polaritons at low densities, below the bosonic condensation threshold, were interpreted as an evidence of strong polariton-polariton interactions [Nat. Phys. 13, 870 (2017)]. In this work, we further investigate the origins of these blueshifts in optically-induced circular traps and present evidence of significant blueshift of the polariton energy due to reshaping of the optically-induced potential with laser pump power. Our work demonstrates strong influence of the effective potential formed by an optically-injected excitonic reservoir on the energy blueshifts observed below and up to the polariton condensation threshold and suggests that the observed blueshifts arise due to interaction of polaritons with the excitonic reservoir, rather than due to polariton-polariton interaction., 10 pages, 8 figures

Bosonic condensates of exciton polaritons (light-matter quasiparticles in a semiconductor) provide a solid-state platform for studies of non-equilibrium quantum systems with a spontaneous macroscopic coherence. These driven, dissipative condensates typically coexist and interact with an incoherent reservoir, which undermines measurements of key parameters of the condensate. Here, we overcome this limitation by creating a high-density exciton-polariton condensate in an optically-induced "box" trap. In this so-called Thomas-Fermi regime, the condensate is fully separated from the reservoir and its behaviour is dominated by interparticle interactions. We use this regime to directly measure the polariton-polariton interaction strength, and reduce the existing uncertainty in its value from four orders of magnitude to within three times the theoretical prediction. The Thomas-Fermi regime has previously been demonstrated only in ultracold atomic gases in thermal equilibrium. In a non-equilibrium exciton-polariton system, this regime offers a novel opportunity to study interaction-driven effects unmasked by an incoherent reservoir., Comment: 11 pages, 5 figures

Integrating monolayers of two-dimensional semiconductors into optical microcavities is challenging because of the very few available approaches to coat the monolayers with dielectric materials without damaging them. Some strategies have been developed, but they either rely on complicated experimental settings and expensive technologies or limit the achievable cavity quality factors. Thus, high quality Fabry–Perot microcavities are not widely available to the community focusing on light-matter coupling in atomically thin materials. Here, we detail a recently developed technique to micro-mechanically assemble Fabry–Perot microcavities. Our approach promotes strong coupling conditions with excitons in atomically thin materials, it does not rely on difficult or expensive technologies, it is reproducible, and it yields microcavities with quality factors approaching 4000. It is ideally suitable for engineering coupled monolayer-cavity systems of advanced complexity in small-scale laboratories.

Atomically thin transition metal dichalcogenide crystals (TMDCs) have extraordinary optical properties that make them attractive for future optoelectronic applications. Integration of TMDCs into practical all-dielectric heterostructures hinges on the ability to passivate and protect them against necessary fabrication steps on large scales. Despite its limited scalability, encapsulation of TMDCs in hexagonal boron nitride (hBN) currently has no viable alternative for achieving high performance of the final device. Here, it is shown that the novel, ultrathin Ga2 O3 glass is an ideal centimeter-scale coating material that enhances optical performance of the monolayers and protects them against further material deposition. In particular, Ga2 O3 capping of monolayer WS2 outperforms commercial-grade hBN in both scalability and optical performance at room temperature. These properties make Ga2 O3 highly suitable for large-scale passivation and protection of monolayer TMDCs in functional heterostructures.

We demonstrate, experimentally and theoretically, controlled loading of an exciton-polariton vortex chain into a 1D array of trapping potentials. Switching between two types of vortex chains, with topological charges of the same or alternating sign, is realised by means of appropriate shaping of an incoherent pump beam that drives the system to the regime of bosonic condensation. In analogy to spin chains, these vortex sequences realise either a "ferromagnetic" or an "anti-ferromagnetic" order, whereby the role of spin is played by the orbital angular momentum. The "ferromagnetic" ordering of vortices is associated with the formation of a persistent chiral current. Our results pave the way for controlled creation of nontrivial distributions of orbital angular momentum and topological order in a periodic exciton-polariton system., 5 pages, 4 figures

A bosonic condensate of exciton polaritons in a semiconductor microcavity is a macroscopic quantum state subject to pumping and decay. The fundamental nature of this driven-dissipative condensate is still under debate. Here, we gain an insight into spontaneous condensation by imaging long-lifetime exciton polaritons in a high-quality inorganic microcavity in a single-shot optical excitation regime, without averaging over multiple condensate realisations. We demonstrate that condensation is strongly influenced by an incoherent reservoir and that the reservoir depletion, the so-called spatial hole burning, is critical for the transition to the ground state. Condensates of photon-like polaritons exhibit strong shot-to-shot fluctuations and density filamentation due to the effective self-focusing associated with the reservoir depletion. In contrast, condensates of exciton-like polaritons display smoother spatial density distributions and are second-order coherent. Our observations show that the single-shot measurements offer a unique opportunity to study fundamental properties of non-equilibrium condensation in the presence of a reservoir.

A bosonic condensate of exciton polaritons in a semiconductor microcavity is a macroscopic quantum state subject to pumping and decay. The fundamental nature of this driven-dissipative condensate is still under debate. Here, we gain an insight into spontaneous condensation by imaging long-lifetime exciton polaritons in a high-quality inorganic microcavity in a single-shot optical excitation regime, without averaging over multiple condensate realisations. We demonstrate that condensation is strongly influenced by an incoherent reservoir and that the reservoir depletion, the so-called spatial hole burning, is critical for the transition to the ground state. Condensates of photon-like polaritons exhibit strong shot-to-shot fluctuations and density filamentation due to the effective self-focusing associated with the reservoir depletion. In contrast, condensates of exciton-like polaritons display smoother spatial density distributions and are second-order coherent. Our observations show that the single-shot measurements offer a unique opportunity to study fundamental properties of non-equilibrium condensation in the presence of a reservoir., The mechanism for exciton-polariton condensation in the presence of an incoherent reservoir has been long debated. Here the authors demonstrate the role of the spatial hole burning in condensation of long‐lived exciton polaritons by imaging the condensates in a single-shot excitation regime.

Publisher's version (útgefin grein), Bosonic condensation belongs to the most intriguing phenomena in physics, and was mostly reserved for experiments with ultra-cold quantum gases. More recently, it became accessible in exciton-based solid-state systems at elevated temperatures. Here, we demonstrate bosonic condensation driven by excitons hosted in an atomically thin layer of MoSe2, strongly coupled to light in a solid-state resonator. The structure is operated in the regime of collective strong coupling between a Tamm-plasmon resonance, GaAs quantum well excitons, and two-dimensional excitons confined in the monolayer crystal. Polariton condensation in a monolayer crystal manifests by a superlinear increase of emission intensity from the hybrid polariton mode, its density-dependent blueshift, and a dramatic collapse of the emission linewidth, a hallmark of temporal coherence. Importantly, we observe a significant spin-polarization in the injected polariton condensate, a fingerprint for spin-valley locking in monolayer excitons. Our results pave the way towards highly nonlinear, coherent valleytronic devices and light sources., We acknowledge fruitful discussions and support on the experiment by Mike Fraser. C.S. acknowledges support by the ERC (Project unLiMIt-2D), and the DFG within the Project SCHN1376 3-1. The Würzburg group acknowledges support by the State of Bavaria. A.N. and E.C. acknowledge the support from the megagrant 14.Y26.31.0015 and Goszadanie no. 3.2614.2017/4.6 of the Ministry of Education and Science of Russian Federation. A.V.K. acknowledges the support from the St-Petersburg State University in framework of the project 11.34.2.2012. S.H. and A.V.K. are grateful for funding received within the EPSRC Hybrid Polaritonics programme grant (EP/M025330/1). S.K. acknowledges the European Commission for the H2020 Marie Skłodowska-Curie Actions fellowship (Topopolis). S.T acknowledges support from NSF DMR 1838443 and NSF DMR 1552220.

We demonstrate generation of chiral modes -- vortex flows with fixed handedness in exciton-polariton quantum fluids. The chiral modes arise in the vicinity of exceptional points (non-Hermitian spectral degeneracies) in an optically-induced resonator for exciton polaritons. In particular, a vortex is generated by driving two dipole modes of the non-Hermitian ring resonator into degeneracy. Transition through the exceptional point in the space of the system's parameters is enabled by precise manipulation of real and imaginary parts of the closed-wall potential forming the resonator. As the system is driven to the vicinity of the exceptional point, we observe the formation of a vortex state with a fixed orbital angular momentum (topological charge). Our method can be extended to generate high-order orbital angular momentum states through coalescence of multiple non-Hermitian spectral degeneracies, which could find application in integrated optoelectronics., 6 pages, 6 figures

Diabolical points (degeneracies) can naturally occur in spectra of two-dimensional quantum systems and classical wave resonators due to simple symmetries. Geometric Berry phase is associated with these spectral degeneracies. Here, we demonstrate a diabolical point and the corresponding Berry phase in the spectrum of hybrid light-matter quasiparticles -- exciton-polaritons in semiconductor microcavities. It is well known that sufficiently strong optical pumping can drive exciton-polaritons to quantum degeneracy, whereby they form a macroscopically populated quantum coherent state similar to a Bose-Einstein condensate. By pumping a microcavity with a spatially structured light, we create a two-dimensional quantum billiard for the exciton-polariton condensate and demonstrate a diabolical point in the spectrum of the billiard eigenstates. The fully reconfigurable geometry of the potential walls controlled by the optical pump enables a striking experimental visualisation of the Berry phase associated with the diabolical point. The Berry phase is observed and measured by direct imaging of the macroscopic exciton-polariton wavefunctions., Comment: 7 pages, 4 figures

We observe degenerate four-wave mixing of exciton-polariton condensates in a semiconductor microcavity in the pulsed non-resonant excitation regime by colliding two counter propagating condensates, which forms an anisotropic halo in k-space.

O.A.E. acknowledges financial support by the Deutsche Forschungsgemeinschaft (DFG project EG344/2-1) and by the EU project (FP7, PIRSES-GA-2013-612600) LIMACONA. I.G.S. acknowledges support from the Academy of Finland through its Centre of Excellence Programs (Projects No. 250280 and No. 251748); Government of Russian Federation (project MK-5903.2016.2); and Dynasty Foundation. E.E., T.G., I.G.S., and E.A.O. acknowledge support by the Australian Research Council. We study the loading of a nonequilibrium, dissipative system of composite bosons - exciton polaritons - into a one dimensional periodic lattice potential. Utilizing momentum resolved photoluminescence spectroscopy, we observe a transition between an incoherent Bose gas and a polariton condensate, which undergoes further transitions between different energy states in the band-gap spectrum of the periodic potential with increasing pumping power. We demonstrate controlled loading into distinct energy bands by modifying the size and shape of the excitation beam. The observed effects are comprehensively described in the framework of a nonequilibrium model of polariton condensation. In particular, we implement a stochastic treatment of quantum and thermal fluctuations in the system and confirm that polariton-phonon scattering is a key energy relaxation mechanism enabling transitions from the highly nonequilibrium polariton condensate in the gap to the ground band condensation for large pump powers. Postprint Postprint

Exciton-polaritons are hybrid light-matter quasiparticles formed by strongly interacting photons and excitons (electron-hole pairs) in semiconductor microcavities. They have emerged as a robust solid-state platform for next-generation optoelectronic applications as well as fundamental studies of quantum many-body physics. Importantly, exciton-polaritons are a profoundly open (i.e., non-Hermitian) quantum system: it requires constant pumping of energy and continuously decays releasing coherent radiation. Thus, the exciton-polaritons always exist in a balanced potential landscape of gain and loss. However, the inherent non-Hermitian nature of this potential has so far been largely ignored in exciton-polariton physics. Here we demonstrate that non-Hermiticity dramatically modifies the structure of modes and spectral degeneracies in exciton-polariton systems, and, therefore, will affect their quantum transport, localisation, and dynamical properties. Using a spatially-structured optical pump, we create a chaotic exciton-polariton billiard. Eigenmodes of this billiard exhibit multiple non-Hermitian spectral degeneracies -- exceptional points. These are known to cause remarkable wave phenomena, such as unidirectional transport, anomalous lasing/absorption, and chiral modes. By varying parameters of the billiard, we observe crossing and anti-crossing of energy levels and reveal the nontrivial topological modal structure exclusive to non-Hermitian systems. We also observe the mode switching and topological Berry phase for a parameter loop encircling the exceptional point. Our findings pave the way for studies of non-Hermitian quantum dynamics of exciton-polaritons, which can lead to novel functionalities of polariton-based devices., Comment: 8 pages, 4 figures