Room temperature topological polariton laser in an organic lattice
Marco Dusel, Simon Betzold, Tristan. H. Harder, Monika Emmerling, Jürgen Ohmer, Utz Fischer, Ronny Thomale, Christian Schneider, Sven Höfling, Sebastian Klembt
Interacting bosonic particles in artificial lattices have proven to be a powerful tool for the investigation of exotic phases of matter as well as phenomena resulting from non-trivial topology. Exciton-polaritons, bosonic quasi-particles of light and matter, have shown to combine the on-chip benefits of optical systems with strong interactions, inherited form their matter character. Technologically significant semiconductor platforms, however, strictly require cryogenic temperatures for operability. In this paper, we demonstrate exciton-polariton lasing for topological defects emerging form the imprinted lattice structure at room temperature. We utilize a monomeric red fluorescent protein derived from DsRed of Discosoma sea anemones, hosting highly stable Frenkel excitons. Using a patterned mirror cavity, we tune the lattice potential landscape of a linear Su-Schrieffer-Heeger chain to design topological defects at domain boundaries and at the edge. In spectroscopic experiments, we unequivocally demonstrate polariton lasing from these topological defects. This progress promises to be a paradigm shift, paving the road to interacting Boson many-body physics at ambient conditions.
Exciton-polaritons are quasiparticles consisting of a linear superposition of photonic and excitonic states, offering potential for nonlinear optical devices. The excitonic component of the polariton provides a finite Coulomb scattering cross section, such that the different types of exciton found in organic materials (Frenkel) and inorganic materials (Wannier-Mott) produce polaritons with different interparticle interaction strength. A hybrid polariton state with distinct excitons provides a potential technological route towards in-situ control of nonlinear behaviour. Here we demonstrate a de…
Exciton-polaritons in semiconductors are quasi-particles which have recently shown the capability to undergo phase transition into a coherent hybrid state of light and matter. The observation of such quasi-particles in organic microcavities has attracted increasing attention for their characteristic of reaching condensation at room temperature. In this work we demonstrate that the emission properties of organic polaritons do not depend on the overlap between the absorption and emission states of the molecule and that the emission dynamics are modified in the strong coupling regime, showing a s…
We demonstrate strong light-matter interaction at ambient conditions between a ladder-type conjugated polymer and the individual modes of a vertical microcavity with tunable resonance frequencies. Zero-dimensional wavelength-scale confinement for the polaritons is achieved through a sub-micron sized Gaussian defect, resulting in a vacuum Rabi splitting of the polariton branches of 2g = 166 meV. By placing a second Gaussian defect nearby, we create a polaritonic molecule with tunnel coupling strength of up to 2J ~ 50 meV. This platform enables the creation of tailor-made potential landscapes wi…
Microcavity-polaritons in two-dimensional lattice geometries have been used to study a wide range of interesting physics. Meanwhile, organic materials have shown great promise on the road towards polaritonic devices, as the strong binding energy of their Frenkel excitons permits room temperature condensation and lasing. Whilst there are theoretical treatments of the condensation processes in planar organic microcavities, models of lattice geometries are lacking. Here, we introduce a model for describing the dynamics of lattices of zero-dimensional organic microcavities, where the dominant cond…
Strongly coupled organic systems are characterized by unusually large Rabi splittings, even in the vacuum state. They show the counter-intuitive feature of a lifetime of the lower polariton state longer than for all other excited states. Here we build up a new theoretical framework to understand the dynamics of such coupled system. In particular, we show that the non-Markovian character of the relaxation of the dressed organic system explains the long lifetime of the lower polariton state.
We report on the origin of energy-shifts in organic polariton condensates. The localised nature of Frenkel excitons in molecular semiconductors precludes interparticle Coulomb exchange interactions -the latter being the dominant mechanism for blueshifts in inorganic semiconductor microcavities that bear Wannier-Mott excitons. We examine the contribution of optically induced change of the intracavity non-linear refractive index, gain induced frequency-pulling and quenching of the Rabi splitting, as well as the role of polariton-exciton and polariton-polariton scattering in the energy-shift of t…
We report on the quantum confinement of zero-dimensional polaritons in perovskite-based microcavity at room temperature. Photoluminescence of discrete polaritonic states are observed for polariton localized in symmetric sphere-like defects which are spontaneously nucleated on the top dielectric Bragg mirror. The linewidth of these confined states are found much sharper (almost one order of magnitude) than that of photonic modes in the perovskite planar microcavity. Our results show the possibility to study organic-inorganic cavity polariton in confined microstructure and suggest a fabrication …
A cavity-polariton, formed due to the strong coupling between exciton and cavity mode, is one of the most promising composite bosons for realizing macroscopic spontaneous coherence at high temperature. Up to date, most of polariton quantum degeneracy experiments were conducted in the complicated two-dimensional (2D) planar microcavities. The role of dimensionality in coherent quantum degeneracy of a composite bosonic system of exciton polaritons remains mysterious. Here we report the first experimental observation of a one-dimensional (1D) polariton condensate in a ZnO microwire at room temper…
In this work electronic structures and optical properties of organic-inorganic exciton and polaritons in two-dimensional heterostructures combining both organic and semiconductor materials are studied. In those systems, Wannier-Frenkel hybrid exciton has unique and interesting properties that can improve the efficiency of optical materials. When an organic-semiconductor combined heterostructure is illuminated by high-intensity electromagnetic radiation with the frequency of the photons at or near the resonance frequency of the Wannier-Frenkel exciton, we obtain a macroscopically occupied syste…
We present a beyond-mean-field approach to predict the nature of organic polariton lasing, accounting for all relevant photon modes in a planar microcavity. Starting from a microscopic picture, we show how lasing can switch between polaritonic states resonant with the maximal gain, and those at the bottom of the polariton dispersion. We show how the population of non-lasing modes can be found, and by using two-time correlations, we show how the photoluminescence spectrum (of both lasing and non-lasing modes) evolves with pumping and coupling strength, confirming recent experimental work on the…
The nonlinear optical response of organic polaritonic matter has received increasing attention due to their enhanced and controllable nonlinear response and their potential for novel optical devices such as compact photon sources and optical and quantum information devices. Using z-scans at different wavelengths and incident powers we have studied the nonlinear optical dispersion of ultrastrongly coupled organic cavity polaritons near the lower polariton band. We show that the up to 150-fold enhancement of the nonlinear response compared to a cavity-less organic film arises from an intensity-d…
The strong-coupling of an excitonic transition with an electromagnetic mode results in composite quasi-particles called exciton-polaritons, which have been shown to combine the best properties of their bare components in semiconductor microcavities. However, the physics and applications of polariton flows in organic materials and at room temperature are still unexplored because of the poor photon confinement in such structures. Here we demonstrate that polaritons formed by the hybridization of organic excitons with a Bloch Surface Wave are able to propagate for hundreds of microns showing rema…
We photo-excite slab polymer waveguides doped with J-aggregating dye molecules and measure the leaky emission from strongly coupled waveguide exciton polariton modes at room temperature. We show that the momentum of the waveguide exciton polaritons can be controlled by modifying the thickness of the excitonic waveguide. Non-resonantly pumped excitons in the slab excitonic waveguide decay into transverse electric and transverse magnetic strongly coupled exciton waveguide modes with radial symmetry. These leak to cones of light with radial and azimuthal polarizations.
Based on the Landauer formalism, we demonstrate that the thermal conductance due to the propagation of surface phonon-polaritons along a polar nanowire is independent of the material characteristics and is given by Pi^2kB^2T/3h. The giant propagation length of these energy carriers establishes that this quantization holds not only for a temperature much smaller than 1 K, as is the case of electrons and phonons, but also for temperatures comparable to room temperature, which can significantly facilitate its observation and application in the thermal management of nanoscale electronics and photo…
Long-range energy transfer in organic molecules has been experimentally obtained by strongly coupling their electronic excitations to a confined electromagnetic cavity mode. Here, we shed light into the polariton-mediated mechanism behind this process for different configurations: donor and acceptor molecules either intermixed or physically separated. We numerically address the phenomenon by means of Bloch-Redfield theory, which allows us to reproduce the effect of complex vibrational reservoirs characteristic of organic molecules. Our findings reveal the key role played by the middle polarito…
We calculate the exact many-body time dynamics of polaritonic states supported by an optical cavity filled with organic molecules. Optical, vibrational and radiative processes are treated on an equal footing employing the Time-Dependent Variational Matrix Product States algorithm. We demonstrate signatures of non-Markovian vibronic dynamics and its fingerprints in the far-field photon emission spectrum at arbitrary light-matter interaction scales, ranging from the weak to the strong coupling regimes. We analyse both the single and many-molecule cases, showing the crucial role played by the col…
In this letter, we address the chiral properties of valley exciton-polaritons in a monolayer of WS2 in the regime of strong light-matter coupling with a Tamm-Plasmon resonance. We observe that the valley polarization, which manifests in the circular polarization of the emitted photoluminescence, is strongly enhanced in comparison to bare WS2 monolayers, and can even be observed under non-resonant excitation at ambient conditions. We study the relaxation and decay dynamics of exciton-polaritons in our device, and present a microscopic model to explain the wave vector-dependent valley depolariza…
Organic microcavities are photonic nanostructures that strongly confine the electromagnetic field, allowing exotic quantum regimes of light-matter interaction with disordered organic semiconductors. The unambiguous interpretation of the spectra of organic microcavities has been a long-standing challenge due to several competing effects involving electrons, vibrations and cavity photons. Here we present a theoretical framework that is able to describe the main spectroscopic features of organic microcavities consistently. We introduce a class of light-matter excitations called dark vibronic pola…
Controlling light-matter interactions in solid-state systems has motivated intense research to produce bosonic quasi-particles known as exciton-polaritons, which requires strong coupling between excitons and cavity photons. Ultra-low threshold coherent light emitters can be achieved through lasing from exciton-polariton condensates, but this generally requires sophisticated device structures and cryogenic temperatures. Polaritonic nanolasers operating at room temperature lie on the crucial path of related research, not only for the exploration of polariton physics at the nanoscale but also for…
Recent experiments on thin-film microcavities give evidence of Bose condensation of exciton-polariton states. Inspired by these observations, we consider the possibility that such exotic "half-light/half matter" states could be observed in thin-film organic semiconductors where the oscillator strength is generally stronger than in inorganic systems. Here we present a theoretical model and simulations of macroscopic exciton-polartiton condensates in thracene thin films sandwiched within a micro-meter scale resonant cavity and establish criteria for the conditions under which BEC could be achiev…
Integrated electro-optical switches are essential as one of the fundamental elements in the development of modern optoelectronics. As an architecture for photonic systems, exciton polaritons, that are hybrid bosonic quasiparticles that possess unique properties derived from both excitons and photons, have shown much promise. For this system, we demonstrate a significant improvement of emitted intensity and condensation threshold by applying an electric field to a microcavity filled with an organic microbelt. Our theoretical investigations indicate that the electric field makes the excitons dip…
We present a microscopic semi-analytical theory for the description of organic molecules interacting strongly with a cavity mode. Exciton-vibration coupling within the molecule and exciton-cavity interaction are treated on an equal footing by employing a temperature-dependent variational approach. The interplay between strong exciton-vibration coupling and strong exciton-cavity coupling gives rise to a hybrid ground state, which we refer to as the lower polaron polariton. Explicit expressions for the ground-state wave function, the zero-temperature quasiparticle weight of the lower polaron pol…
Starting from a microscopic model, we investigate the optical spectra of molecules in strongly-coupled organic microcavities examining how they might self-consistently adapt their coupling to light. We consider both rotational and vibrational degrees of freedom, focusing on features which can be seen in the peak in the center of the spectrum at the bare excitonic frequency. In both cases we find that the matter-light coupling can lead to a self-consistent change of the molecular states, with consequent temperature-dependent signatures in the absorption spectrum. However, for typical parameters…
Exciton-polaritons are quasiparticles with mixed photon and exciton character that demonstrate rich quantum phenomena, novel optoelectronic devices and the potential to modify chemical properties of materials. Organic semiconductors are of current interest for their room-temperature polariton formation. However, within organic optoelectronic devices, it is often the 'dark' spin-1 triplet excitons that dominate operation. These triplets have been largely ignored in treatments of polariton physics. Here we demonstrate polariton population from the triplet manifold via triplet-triplet annihilatio…
Exciton-polaritons (polaritons herein) in transition-metal dichalcogenide monolayers have attracted significant attention due to their potential for polariton-based optoelectronics. Many of the proposed applications rely on the ability to trap polaritons and to reach macroscopic occupation of their ground energy state. Here, we engineer a trap for room-temperature polaritons in an all-dielectric optical microcavity by locally increasing the interactions between the WS$_2$ excitons and cavity photons. The resulting confinement enhances the population and the first-order coherence of the polarit…
We embedded an all-hydrocarbon-based carbocation in a metallic microcavity that was tuned to resonance with an electronic transition of the carbocation. The measured Rabi splitting was 41% of the excitation energy, putting the system well into the ultrastrong coupling regime. Importantly, due to the intrinsic charge on the carbocation, the polaritons that form carry a significant charge fraction $0.55 e_0$ and a large charge-to-mass ratio ($\sim 2400 e_0 / m_0$). Moreover, the ground state of the ultrastrongly coupled system is calculated to carry about one percent of one elementary charge, im…
Magnetic and spin-based technologies for data storage and processing pose unique challenges for information transduction to light because of magnetic metals' optical loss, and the inefficiency and resistivity of semiconductor spin-based emitters at room temperature. Transduction between magnetic and optical information in typical organic semiconductors poses additional challenges as the Faraday and Kerr magnetooptical effects rely on the electronic spin-orbit interaction, and the spin-orbit interaction in organics is weak. Other methods of coupling light and spin have emerged in organics, howe…
Polaritons are hybrid light-matter quasi-particles that have gathered a significant attention for their capability to show room temperature and out-of-equilibrium Bose-Einstein condensation. More recently, a novel class of ultrafast optical devices have been realized by using flows of polariton fluids, such as switches, interferometers and logical gates. However, polariton lifetimes and propagation distance are strongly limited by photon losses and accessible in-plane momenta in usual microcavity samples. In this work, we show experimental evidence of the formation of room temperature propagat…
Exciton-polaritons in semiconductor microcavities generate fascinating effects such as long-range spatial coherence and Bose-Einstein Condensation (BEC), which are attractive for their potential use in low threshold lasers, vortices and slowing light, etc. However, currently most of exciton-polariton effects either occur at cryogenic temperature or rely on expensive cavity fabrication procedures. Further exploring new semiconductor microcavities with stronger exciton photon interaction strength is extensively needed. Herein, we demonstrate room temperature photon exciton strong coupling in hyb…
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…
Hybrid halide perovskites are now considered as low-cost materials for contemporary research in photovoltaics and nanophotonics. In particular, because these materials can be solution processed, they represent a great hope for obtaining low-cost devices. While the potential of 2D layered hybrid perovskites for polaritonic devices operating at room temperature has been demonstrated in the past, the potential of the 3D perovskites has been much less explored for this particular application. Here, we report the strong exciton-photon coupling with 3D bromide hybrid perovskite. Cavity polaritons ar…
We review the recent developments of the polariton physics in microcavities featuring the exciton-photon strong coupling at room-temperature, and leading to the achievement of room-temperature polariton condensates. Such cavities embed active layers with robust excitons that present a large binding energy and a large oscillator strength, i.e. wide bandgap inorganic or organic semiconductors, or organic molecules. These various systems are compared, in terms of figures of merit and of common features related to their strong oscillator strength. The various demonstrations of polariton laser are …
Monolayered MoSe2 is a promising new material to investigate advanced light-matter coupling as it hosts stable and robust excitons with comparably narrow optical resonances. In this work, we investigate the evolution of the lowest lying excitonic transition, the so-called A-valley exciton, with temperature. We find a strong, phonon-induced temperature broadening of the resonance, and more importantly, a reduction of the oscillator strength for increased temperatures. Based on these experimentally extracted, temperature dependent parameters, we apply a coupled oscillator model to elucidate the …
A new platform for fabricating polariton lasers operating at room temperature is introduced: nitride-based distributed Bragg reflectors epitaxially grown on patterned silicon substrates. The patterning allows for an enhanced strain relaxation thereby enabling to stack a large number of crack-free AlN/AlGaN pairs and achieve cavity quality factors of several thousands with a large spatial homogeneity. GaN and ZnO active regions are epitaxially grown thereon and the cavities are completed with top dielectric Bragg reflectors. The two structures display strong-coupling and polariton lasing at roo…
By considering driven diffusive dynamics of exciton polaritons in an optical microcavity with an embedded molybdenum disulfide monolayer, we determine experimentally relevant range of parameters at which room-temperature superfuidity can be observed. It is shown that the superfluid transitions occurs in a trapped polariton gas at laser pumping power $P>600$ mW and and trapping potential strength $k > 50$ eV/cm$^2$. We also propose a simple analytic model that provides a useful estimate for the polariton gas density, which enables one to determine the conditions for observation of room temperat…
We explore the generation of anti-Stokes fluorescence from strongly coupled organic dye microcavities following resonant ground-state excitation. We observe polariton emission along the lower polariton branch, with our results indicating that this process involves a return to the exciton reservoir and the absorption of thermal energy from molecules in a vibrationally excited ground-state. We speculate that the generation of a population of "hot" polaritons is enhanced by the fact that the cavity supresses the emission of Stokes-shifted fluorescence, as it is located energetically below the cut…
Exciton-polaritons resulting from the strong exciton-photon interaction stimulate the development of novel coherent light sources with low threshold, long range spatial, and temporal coherence to circumvent the ever increasing energy demands of optical communications. Polaritons from bound states in the continuum (BICs) are promising for Bose-Einstein condensation owing to their infinite quality factors that enlarge photon lifetimes and benefit polariton accumulations. However, BIC polariton condensation remains limited to cryogenic temperatures ascribed to the small exciton binding energies o…
Semiconductor microcavity polaritons, formed via strong exciton-photon coupling, provide a quantum many-body system on a chip, featuring rich physics phenomena for better photonic technology. However, conventional polariton cavities are bulky, difficult to integrate, and inflexible for mode control, especially for room temperature materials. Here we demonstrate sub-wavelength thick one-dimensional photonic crystals (PCs) as a designable, compact and practical platform for strong coupling with atomically thin van der Waals Crystals (vdWCs). Polariton dispersions and mode anti-crossings are meas…
Atomically-thin transition metal dichalcogenide crystals (TMDCs) hold great promise for future semiconductor optoelectronics due to their unique electronic and optical properties. In particular, electron-hole pairs (excitons) in TMDCs are stable at room temperature and interact strongly with light. When TMDCs are embedded in an optical microcavity, the excitons can hybridise with cavity photons to form exciton polaritons (polaritons herein), which display both ultrafast velocities and strong interactions. The ability to manipulate and trap polaritons on a microchip is critical for future appli…
Here we report the fabrication and optical characterization of organic microcavities containing liquid-crystalline conjugated polymers (LCCPs): poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT), poly(9,9-dioctylfluorene) (PFO) and poly(2,7-(9,9-dihexylfluorene)-co-bithiophene) (F6T2) aligned on top of a thin transparent Sulfuric Dye 1 (SD1) photoalignment layer. We extract the optical constants of the aligned films using variable angle spectroscopic ellipsometry and fabricate metallic microcavities in which the ultrastrong coupling regime is manifest both for the aligned and non-aligned LCC…
We study the dynamics of multimode polariton lasing in organic microcavities by using a second-order cumulant equation approach. By inspecting the time evolution of the photon mode occupations, we show that if multiple lasing peaks are observed in time-integrated mode occupations, the reason can be either bi-modal lasing or temporal switching between several modes. The former takes place within a narrow range of parameters while the latter occurs more widely. We find that the origin of the temporal switching is different in the weak- and strong-coupling regimes. At weak coupling slope efficien…
We report measurement of the ensemble averaged transverse spin relaxation time (T2*) in bulk and few molecules of the organic semiconductor tris(8-hydroxyquinolinolato aluminum) or Alq3. This system exhibits two characteristic T2* times, the longer of which is temperature-independent and the shorter is temperature-dependent, indicating that the latter is most likely limited by spin-phonon interaction. Based on the measured data, we infer that the single particle T2 time is long enough to meet Knill's criterion for fault tolerant quantum computing, even at room temperature. Alq3 is also an opti…
We create exciton-polaritons in a zero-dimensional (0D) microcavity filled with organic ladder-type conjugated polymer in the strong light-matter interaction regime. Photonic confinement at wavelength scale is realized in the longitudinal direction by two dielectric Bragg mirrors and laterally by a sub-micron Gaussian-shaped defect. The cavity is separated into two parts allowing nanometer position control and enabling tuning of exciton and photon fractions of the polariton wavefunction. Polariton condensation is achieved with non-resonant, picosecond optical excitation at ambient conditions a…
In the field of spin-controlled semiconductor lasers, massive effort has been focused upon materials with long spin relaxation times (~ns). In contrast, we demonstrate room-temperature spin-polarized ultrafast pulsed lasing in InGaAs quantum wells (~10 ps) embedded within a GaAs microcavity. The microcavity studied here is similar to vertical-cavity surface-emitting lasers (VCSEL) used in optical communication. Unlike a VCSEL, the present polariton laser has nonlinear output and energy shifts owing to the mixing of the free-carrier polarization and cavity light field. At room temperature, we o…
Whispering gallery modes in a microwire are characterized by a nearly equidistant energy spectrum. In the strong exciton-photon coupling regime, this system represents a bosonic cascade: a ladder of discrete energy levels that sustains stimulated transitions between neighboring steps. In this work, by using femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity is explicitly visualized. Clear ladder-form build-up process from higher to lower energy branches of the polari…
