Strong Exciton-photon Coupling Regime Research Articles

Quantitative Investigation of the Rate of Intersystem Crossing in the Strong Exciton-Photon Coupling Regime.

Strong interactions between excitons and photons lead to the formation of exciton-polaritons, which possess completely different properties compared to their constituents. The polaritons are created by incorporating a material in an optical cavity where the electromagnetic field is tightly confined. Over the last few years, the relaxation of polaritonic states has been shown to enable a new kind of energy transfer event, which is efficient at length scales substantially larger than the typical Förster radius. However, the importance of such energy transfer depends on the ability of the short-lived polaritonic states to efficiently decay to molecular localized states that can perform a photochemical process, such as charge transfer or triplet states. Here, we investigate quantitatively the interaction between polaritons and triplet states of erythrosine B in the strong coupling regime. We analyze the experimental data, collected mainly employing angle-resolved reflectivity and excitation measurements, using a rate equation model. We show that the rate of intersystem crossing from the polariton to the triplet states depends on the energy alignment of the excited polaritonic states. Furthermore, it is demonstrated that the rate of intersystem crossing can be substantially enhanced in the strong coupling regime to the point where it approaches the rate of the radiative decay of the polariton. In light of the opportunities that transitions from polaritonic to molecular localized states offer within molecular photophysics/chemistry and organic electronics, we hope that the quantitative understanding of such interactions gained from this study will aid in the development of polariton-empowered devices.

Polariton lasing in AlGaN microring with GaN/AlGaN quantum wells

Microcavity polaritons are strongly interacting hybrid light–matter quasiparticles, which are promising for the development of novel light sources and active photonic devices. Here, we report polariton lasing in the UV spectral range in microring resonators based on GaN/AlGaN slab waveguides, with experiments carried out from 4 K up to room temperature. Stimulated polariton relaxation into multiple ring resonator modes is observed, which exhibit threshold-like dependence of the emission intensity with pulse energy. The strong exciton-photon coupling regime is confirmed by the significant reduction of the free spectral range with energy and the blueshift of the exciton–like modes with increasing pulse energy. Importantly, the exciton emission shows no broadening with power, further confirming that lasing is observed at electron–hole densities well below the Mott transition. Overall, our work paves the way toward the development of novel UV devices based on the high-speed slab waveguide polariton geometry operating up to room temperature with the potential to be integrated into complex photonic circuits.

Enhanced Cavity Optomechanics with Quantum-Well Exciton Polaritons.

Semiconductor microresonators embedding quantum wells can host tightly confined and mutually interacting excitonic, optical, and mechanical modes at once. We theoretically investigate the case where the system operates in the strong exciton-photon coupling regime, while the optical and excitonic resonances are parametrically modulated by the interaction with a mechanical mode. Owing to the large exciton-phonon coupling at play in semiconductors, we predict an enhancement of polariton-phonon interactions by 2 orders of magnitude with respect to mere optomechanical coupling: a near-unity single-polariton quantum cooperativity is within reach for current semiconductor resonator platforms. We further analyze how polariton nonlinearities affect dynamical backaction, modifying the capability to cool or amplify the mechanical motion.

Femtosecond Dynamics of a Polariton Bosonic Cascade at Room Temperature.

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. Here, by using a femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity are explicitly visualized. Clear ladder-form build-up processes from higher to lower energy branches of the polariton condensates are observed, which are well reproduced by modeling using rate equations. Remarkably, a pronounced superbunching feature, which could serve as solid evidence for bosonic cascades, is demonstrated by the measured second-order time correlation factor. In addition, the nonlinear polariton parametric scattering dynamics on a time scale of hundreds of femtoseconds are revealed. Our understandings pave the way toward ultrafast coherent control of polaritons at room temperature.

Strong exciton-photon coupling in large area MoSe2 and WSe2 heterostructures fabricated from two-dimensional materials grown by chemical vapor deposition

Two-dimensional semiconducting transition metal dichalcogenides embedded in optical microcavities in the strong exciton-photon coupling regime may lead to promising applications in spin and valley addressable polaritonic logic gates and circuits. One significant obstacle for their realization is the inherent lack of scalability associated with the mechanical exfoliation commonly used for fabrication of two-dimensional materials and their heterostructures. Chemical vapor deposition offers an alternative scalable fabrication method for both monolayer semiconductors and other two-dimensional materials, such as hexagonal boron nitride. Observation of the strong light-matter coupling in chemical vapor grown transition metal dichalcogenides has been demonstrated so far in a handful of experiments with monolayer molybdenum disulfide and tungsten disulfide. Here we instead demonstrate the strong exciton-photon coupling in microcavities composed of large area transition metal dichalcogenide/hexagonal boron nitride heterostructures made from chemical vapor deposition grown molybdenum diselenide and tungsten diselenide encapsulated on one or both sides in continuous few-layer boron nitride films also grown by chemical vapor deposition. These transition metal dichalcogenide/hexagonal boron nitride heterostructures show high optical quality comparable with mechanically exfoliated samples, allowing operation in the strong coupling regime in a wide range of temperatures down to 4 Kelvin in tunable and monolithic microcavities, and demonstrating the possibility to successfully develop large area transition metal dichalcogenide based polariton devices.

Entropic Mixing Allows Monomeric-Like Absorption in Neat BODIPY Films.

Intermolecular interactions play a crucial role in materials chemistry because they govern thin film morphology. The photophysical properties of films of organic dyes are highly sensitive to the local environment, and a considerable effort has therefore been dedicated to engineering the morphology of organic thin films. Solubilizing side chains can successfully spatially separate chromophores, reducing detrimental intermolecular interactions. However, this strategy is also significantly decreasing achievable dye concentration. Here, five BODIPY derivatives containing small alkyl chains in the α‐position were synthesized and photophysically characterized. By blending two or more derivatives, the increase in entropy reduces aggregation and therefore produces films with extreme dye concentration and, at the same time almost solution like absorption properties. Such a film was placed inside an optical cavity and the achieved system was demonstrated to reach the strong exciton‐photon coupling regime by virtue of the achieved dye concentration and sharp absorption features of the film.

Hybrid optical fiber for light-induced superconductivity

We exploit the recent proposals for the light-induced superconductivity mediated by a Bose-Einstein condensate of exciton-polaritons to design a superconducting fiber that would enable long-distance transport of a supercurrent at elevated temperatures. The proposed fiber consists of a conventional core made of a silica glass with the first cladding layer formed by a material sustaining dipole-polarised excitons with a binding energy exceeding 25 meV. To be specific, we consider a perovskite cladding layer of 20 nm width. The second cladding layer is made of a conventional superconductor such as aluminium. The fiber is covered by a conventional coating buffer and by a plastic outer jacket. We argue that the critical temperature for a superconducting phase transition in the second cladding layer may be strongly enhanced due to the coupling of the superconductor to a bosonic condensate of exciton-polaritons optically induced by the evanescent part of the guiding mode confined in the core. The guided light mode would penetrate to the first cladding layer and provide the strong exciton-photon coupling regime. We run simulations that confirm the validity of the proposed concept. The fabrication of superconducting fibers where a high-temperature superconductivity could be controlled by light would enable passing superconducting currents over extremely long distances.

A Nanophotonic Structure Containing Living Photosynthetic Bacteria.

Photosynthetic organisms rely on a series of self-assembled nanostructures with tuned electronic energy levels in order to transport energy from where it is collected by photon absorption, to reaction centers where the energy is used to drive chemical reactions. In the photosynthetic bacteria Chlorobaculum tepidum, a member of the green sulfur bacteria family, light is absorbed by large antenna complexes called chlorosomes to create an exciton. The exciton is transferred to a protein baseplate attached to the chlorosome, before migrating through the Fenna-Matthews-Olson complex to the reaction center. Here, it is shown that by placing living Chlorobaculum tepidum bacteria within a photonic microcavity, the strong exciton-photon coupling regime between a confined cavity mode and exciton states of the chlorosome can be accessed, whereby a coherent exchange of energy between the bacteria and cavity mode results in the formation of polariton states. The polaritons have energy distinct from that of the exciton which can be tuned by modifying the energy of the optical modes of the microcavity. It is believed that this is the first demonstration of the modification of energy levels within living biological systems using a photonic structure.

Microcavity controlled coupling of excitonic qubits

Controlled non-local energy and coherence transfer enables light harvesting in photosynthesis and non-local logical operations in quantum computing. This process is intuitively pictured by a pair of mechanical oscillators, coupled by a spring, allowing for a reversible exchange of excitation. On a microscopic level, the most relevant mechanism of coherent coupling of distant quantum bits—like trapped ions, superconducting qubits or excitons confined in semiconductor quantum dots—is coupling via the electromagnetic field. Here we demonstrate the controlled coherent coupling of spatially separated quantum dots via the photon mode of a solid state microresonator using the strong exciton–photon coupling regime. This is enabled by two-dimensional spectroscopy of the sample’s coherent response, a sensitive probe of the coherent coupling. The results are quantitatively understood in a rigorous description of the cavity-mediated coupling of the quantum dot excitons. This mechanism can be used, for instance in photonic crystal cavity networks, to enable a long-range, non-local coherent coupling.

Control of polariton scattering in resonant-tunneling double-quantum-well semiconductor microcavities

Electronic control of ultrafast optical amplification is achieved in specially designed semiconductor microcavities with double quantum well. The gain from parametric scattering of polaritons is selectively quenched by tuning the intracavity electric field to turn on and off interwell resonant tunneling. A $>90\mathrm{%}$ reduction in optical gain is observed with only 100 mV change in applied bias. The strong exciton-photon coupling regime leads here to competition between the rate of Rabi coupling and of electronic tunneling between adjacent quantum wells.

In-gap polaritons in uniformly filled microcavities

We examine the nature and the dispersion of new polariton modes, which appear in thepolariton gap (i.e. within the Rabi splitting), considering the spectrum of polaritons in aplanar microcavity uniformly filled with a resonant material and exhibiting the strongexciton–photon coupling regime. These additional modes are the consequence of thequantization of the excitonic states caused by the confinement. We consider these in-gapmodes in materials typically used in microcavities and link the obtained results toexperiments, where such in-gap states have indeed been observed. We show that thesplitting between the in-gap modes and their bandwidth depend on the bandwidth of theexciton out of the microcavity and on the oscillator strength of the excitonic transition.

Coupling of polaritons to vibrational modes of ultracold atoms in an optical lattice

The coupling of internal electronic excitations to vibrational modes of the external motion of ultracold atoms in an optical lattice is studied here in using a perturbation expansion in small atomic displacements. In the Mott insulator case with one atom per site, the resonance dipole–dipole coupling between neighboring sites can induce emission and absorption of vibrational quanta. Within a cavity in the strong exciton–photon coupling regime such coupling results in polariton–vibration interactions, which create a significant thermalization mechanism for polaritons toward their minimum energy, and leading to motional heating of the lattice atoms.

Strong exciton-photon coupling in ZnO based resonators

The authors report on the fabrication of high quality all-oxide Bragg reflectors (BRs) and ZnO based resonators. The resonator consists of a bulk half-wavelength ZnO microcavity embedded between two BRs, each made of 10.5 layer pairs of yttria stabilized zirconia and Al2O3. Scanning transmission electron microscopy and atomic force microscopy, yield smooth interfaces and low surface roughness for the BR as well as the resonator. For the BR with 10.5 layer pairs the authors obtain reflectivities up to 99.2% within the Bragg stop band. The exciton-polariton dispersion was determined by both, polarization- and angle-resolved photoluminescence (PL) and reflectivity (R) measurements. The detuning between the uncoupled exciton mode and photon mode was changed by shifting the exciton mode energy in the temperature range of 10–290 K. Thereby we observed that a strong exciton-photon coupling regime up to room temperature is present in our resonators with maximum values of the Rabi splitting of about 68 meV (PL, T=10 K) and 76 meV (R,T=10 K).

Goldstone mode of optical parametric oscillators in planar semiconductor microcavities in the strong-coupling regime

We propose an experimental setup to probe the low-lying excitation modes of a parametrically oscillating planar cavity, in particular the soft Goldstone mode which appears as a consequence of the spontaneously broken $\text{U}(1)$ symmetry of signal-idler phase rotations. A strong and narrow peak corresponding to the Goldstone mode is identified in the transmission spectrum of a weak probe beam incident on the cavity. When the $\text{U}(1)$ symmetry is explicitly broken by an additional laser beam pinning the signal-idler phase, a gap opens in the dispersion and the Goldstone peak is dramatically suppressed. Quantitative predictions are given for the case of semiconductor planar cavities in the strong exciton-photon coupling regime.

Quantum Monte Carlo study of ring-shaped polariton parametric luminescence in a semiconductor microcavity

We present a quantum Monte Carlo study of the quantum correlations in the parametric luminescence from semiconductor microcavities in the strong exciton-photon coupling regime. As already demonstrated in recent experiments, a ring-shaped emission is obtained by applying two identical pump beams with opposite in-plane wavevectors, providing symmetrical signal and idler beams with opposite in-plane wavevectors on the ring. We study the squeezing of the signal-idler difference noise across the parametric instability threshold, accounting for the radiative and non-radiative losses, multiple scattering and static disorder. We compare the results of the complete multimode Monte Carlo simulations with a simplified linearized quantum Langevin analytical model.

Absence of long-range coherence in the parametric emission of photonic wires

We analytically investigate the spatial coherence properties of the signal emission from one-dimensional optical parametric oscillators. Because of the reduced dimensionality, quantum fluctuations are able to destroy the long-range phase coherence even far above threshold. The spatial decay of coherence is exponential and, for realistic parameters of semiconductor photonic wires in the strong exciton-photon coupling regime, it is predicted to occur on an experimentally accessible length scale.

Polariton quantum blockade in a photonic dot

We investigate the quantum nonlinear dynamics of a resonantly excited photonic quantum dot embedding a quantum well in the strong exciton-photon coupling regime. Within a master equation approach, we study the polariton quantum blockade and the generation of single photon states due to polariton-polariton interactions as a function of the photonic dot geometry, spectral linewidths and energy detuning between quantum well exciton and confined photon mode. The second order coherence function $g^{(2)}(t,t')$ is calculated for both continuous wave and pulsed excitations.

Evidence of polariton-induced transparency in a single organic quantum wire

The resonant interaction between quasi-one dimensional excitons and photons is investigated. For a single isolated organic quantum wire, embedded in its single crystal monomer matrix, the strong exciton-photon coupling regime is reached. This is evidenced by the suppression of the resonant excitonic absorption arising when the system eigenstate is a polariton. These observations demonstrate that the resonant excitonic absorption in a semiconductor can be understood in terms of a balance between the exciton coherence time and the Rabi period between exciton-like and photon-like states of the polariton.

Polariton quantum boxes in semiconductor microcavities

We report on the realization of polariton quantum boxes in a semiconductor microcavity under strong coupling regime. The quantum boxes consist of mesas, etched on the top of the spacer of a microcavity, that confine the cavity photon. For mesas with sizes of the order of a few microns in width and nanometers in depth, we observe quantization of the polariton modes in several states, caused by the lateral confinement. We evidence the strong exciton-photon coupling regime through a typical anticrossing curve for each quantized level. Moreover, the growth technique permits one to obtain high-quality samples, and opens the way for the conception of new optoelectronic devices.

Spontaneous Coherent Phase Transition of Polaritons in CdTe Microcavities

We report on evidence for polariton condensation out of a reservoir of incoherent polaritons. Polariton population and first-order coherence are investigated by spectroscopic imaging of the far-field emission of a CdTe-based microcavity under nonresonant pumping. With increasing pumping power, stimulated emission with thresholdlike behavior and spectral narrowing is observed in the strong exciton-photon coupling regime. We show that it comes from a narrow ring in k space, exhibiting enhanced spatial and angular coherence at the stimulation onset.