Lucas C. Flatten

Room-temperature exciton-polaritons with two-dimensional WS2

Two-dimensional transition metal dichalcogenides exhibit strong optical transitions with significant potential for optoelectronic devices. In particular they are suited for cavity quantum electrodynamics in which strong coupling leads to polariton formation as a root to realisation of inversionless lasing, polariton condensation and superfluidity. Demonstrations of such strongly correlated phenomena to date have often relied on cryogenic temperatures, high excitation densities and were frequently impaired by strong material disorder. At room-temperature, experiments approaching the strong coupling regime with transition metal dichalcogenides have been reported, but well resolved exciton-polaritons have yet to be achieved. Here we report a study of monolayer WS2 coupled to an open Fabry-Perot cavity at room-temperature, in which polariton eigenstates are unambiguously displayed. In-situ tunability of the cavity length results in a maximal Rabi splitting of ħΩRabi = 70 meV, exceeding the exciton linewidth. Our data are well described by a transfer matrix model appropriate for the large linewidth regime. This work provides a platform towards observing strongly correlated polariton phenomena in compact photonic devices for ambient temperature applications.

Strong Exciton-Photon Coupling with Colloidal Nanoplatelets in an Open Microcavity.

Colloidal semiconductor nanoplatelets exhibit quantum size effects due to their thickness of only a few monolayers, together with strong optical band-edge transitions facilitated by large lateral extensions. In this article, we demonstrate room temperature strong coupling of the light and heavy hole exciton transitions of CdSe nanoplatelets with the photonic modes of an open planar microcavity. Vacuum Rabi splittings of 66 ± 1 meV and 58 ± 1 meV are observed for the heavy and light hole excitons, respectively, together with a polariton-mediated hybridization of both transitions. By measuring the concentration of platelets in the film, we compute the transition dipole moment of a nanoplatelet exciton to be μ = (575 ± 110) D. The large oscillator strength and fluorescence quantum yield of semiconductor nanoplatelets provide a perspective toward novel photonic devices by combining polaritonic and spinoptronic effects.

Electrically tunable organic-inorganic hybrid polaritons with monolayer WS2.

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 device in which hybrid polaritons are displayed at ambient temperatures, the excitonic component of which is part Frenkel and part Wannier-Mott, and in which the dominant exciton type can be switched with an applied voltage. The device consists of an open microcavity containing both organic dye and a monolayer of the transition metal dichalcogenide WS2. Our findings offer a perspective for electrically controlled nonlinear polariton devices at room temperature.

Spectral engineering of coupled open‐access microcavities

Open-access microcavities are emerging as a new approach to confine and engineer light at mode volumes down to the λ3 regime. They offer direct access to a highly confined electromagnetic field while maintaining tunability of the system and flexibility for coupling to a range of matter systems. This article presents a study of coupled cavities, for which the substrates are produced using Focused Ion Beam milling. Based on experimental and theoretical investigation the engineering of the coupling between two microcavities with radius of curvature of 6 inline imagem is demonstrated. Details are provided by studying the evolution of spectral, spatial and polarisation properties through the transition from isolated to coupled cavities. Normal mode splittings up to 20 meV are observed for total mode volumes around inline image. This work is of importance for future development of lab-on-a-chip sensors and photonic open-access devices ranging from polariton systems to quantum simulators.

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 (Cba. tepidum), a member of the green sulphur bacteria (GSB) family, light is absorbed by large antenna complexes called chlorosomes. The exciton generated is transferred to a protein baseplate attached to the chlorosome, before traveling through the Fenna-Matthews-Olson (FMO) complex to the reaction center. The energy levels of these systems are generally defined by their chemical structure. Here we show that by placing bacteria within a photonic microcavity, we can access the strong exciton-photon coupling regime between a confined cavity mode and exciton states of the chlorosome, whereby a coherent exchange of energy between the bacteria and cavity mode results in the formation of polariton states. The polaritons have an energy distinct from that of the exciton and photon, and can be tuned in situ via the microcavity length. This results in real-time, non-invasive control over the relative energy levels within the bacteria. This demonstrates the ability to strongly influence living biological systems with photonic structures such as microcavities. We believe that by creating polariton states, that are in this case a superposition of a photon and excitons within a living bacteria, we can modify energy transfer pathways and therefore study the importance of energy level alignment on the efficiency of photosynthetic systems.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.

Driven-dissipative non-equilibrium Bose–Einstein condensation of less than ten photons

In a Bose–Einstein condensate, bosons condense in the lowest-energy mode available and exhibit high coherence. Quantum condensation is inherently a multimode phenomenon, yet understanding of the condensation transition in the macroscopic limit is hampered by the difficulty in resolving populations of individual modes and the coherences between them. Here, we report non-equilibrium Bose–Einstein condensation of 7 ± 2 photons in a sculpted dye-filled microcavity, where the extremely small particle number and large mode spacing of the condensate allow us to measure occupancies and coherences of the individual energy levels of the bosonic field. Coherence of the individual modes is found to generally increase with increasing photon number. However, at the break-down of thermal equilibrium we observe phase transitions to a multimode condensate regime wherein coherence unexpectedly decreases with increasing population, suggesting the presence of strong intermode phase or number correlations despite the absence of a direct nonlinearity. Experiments are well-matched to a detailed non-equilibrium model. We find that microlaser and Bose–Einstein statistics each describe complementary parts of our data and are limits of our model in appropriate regimes, providing elements to inform the debate on the differences between the two concepts1,2.Non-equilibrium Bose–Einstein condensation of 7 ± 2 photons is observed in a sculpted dye-filled microcavity. The small number of particles allows the authors to access and characterize the non-equilibrium dynamics of the bosonic modes.