Christof P. Dietrich

An exciton-polariton laser based on biologically produced fluorescent protein

Microcavities filled with biologically produced green fluorescent protein show polariton condensation at room temperature. Under adequate conditions, cavity polaritons form a macroscopic coherent quantum state, known as polariton condensate. Compared to Wannier-Mott excitons in inorganic semiconductors, the localized Frenkel excitons in organic emitter materials show weaker interaction with each other but stronger coupling to light, which recently enabled the first realization of a polariton condensate at room temperature. However, this required ultrafast optical pumping, which limits the applications of organic polariton condensates. We demonstrate room temperature polariton condensates of cavity polaritons in simple laminated microcavities filled with biologically produced enhanced green fluorescent protein (eGFP). The unique molecular structure of eGFP prevents exciton annihilation even at high excitation densities, thus facilitating polariton condensation under conventional nanosecond pumping. Condensation is clearly evidenced by a distinct threshold, an interaction-induced blueshift of the condensate, long-range coherence, and the presence of a second threshold at higher excitation density that is associated with the onset of photon lasing.

Room-temperature Tamm-plasmon exciton-polaritons with a WSe2 monolayer.

Solid-state cavity quantum electrodynamics is a rapidly advancing field, which explores the frontiers of light–matter coupling. Metal-based approaches are of particular interest in this field, as they carry the potential to squeeze optical modes to spaces significantly below the diffraction limit. Transition metal dichalcogenides are ideally suited as the active material in cavity quantum electrodynamics, as they interact strongly with light at the ultimate monolayer limit. Here, we implement a Tamm-plasmon-polariton structure and study the coupling to a monolayer of WSe2, hosting highly stable excitons. Exciton-polariton formation at room temperature is manifested in the characteristic energy–momentum dispersion relation studied in photoluminescence, featuring an anti-crossing between the exciton and photon modes with a Rabi-splitting of 23.5u2009meV. Creating polaritonic quasiparticles in monolithic, compact architectures with atomic monolayers under ambient conditions is a crucial step towards the exploration of nonlinearities, macroscopic coherence and advanced spinor physics with novel, low-mass bosons.

Multi-state lasing in self-assembled ring-shaped green fluorescent protein microcavities

We demonstrate highly efficient lasing from multiple photonic states in microcavities filled with self-assembled rings of recombinant enhanced green fluorescent protein (eGFP) in its solid state form. The lasing regime is achieved at very low excitation energies of 13 nJ and occurs from cavity modes dispersed in both energy and momentum. We attribute the momentum distribution to very efficient scattering of incident light at the surface of the eGFP rings. The distribution of lasing states in energy is induced by the large spectral width of the gain spectrum of recombinant eGFP (FWHM ≅ 25u2009nm).

Influence of optical material properties on strong coupling in organic semiconductor based microcavities

The optical properties of organic semiconductors are generally characterised by a number of material specific parameters, including absorbance, photoluminescence quantum yield, Stokes shift, and molecular orientation. Here, we study four different organic semiconductors and compare their optical properties to the characteristics of the exciton-polaritons that are formed when these materials are introduced into metal-clad microcavities. We find that the strength of coupling between cavity photons and excitons is clearly correlated with the absorptivity of the material. In addition, we show that anisotropy strongly affects the characteristics of the formed exciton-polaritons.

Optofluidic distributed feedback lasers with evanescent pumping: Reduced threshold and angular dispersion analysis

We demonstrate an evanescently pumped water-based optofluidic distributed feedback (DFB) laser with a record low pump threshold of ETH=520u2009nJ. The low threshold results from an optimized mode shape, which is achieved by a low refractive index substrate, and from the use of a mixed-order DFB grating. Investigating the photonic band structure via angular dispersion analysis both above and below lasing threshold allows us to measure the refractive index of the liquid gain layer and to determine the device parameters such as the waveguide core layer thickness. We show that it is possible to tailor the divergence of the lasing emission by varying the number of second order grating periods used for outcoupling.

Molding Photonic Boxes into Fluorescent Emitters by Direct Laser Writing

Direct laser writing of photonic boxes into active layers of biologically produced recombinant fluorescent protein in optical microcavities is demonstrated. Irradiation with laser light above the photobleaching threshold induces photonic confinement potentials on the order of 40 meV. The technique provides high spatial selectivity and enables room-temperature lasing in protein rings, and circular and elliptical pillars with customized beam shapes.

Room temperature strong coupling in a semiconductor microcavity with embedded AlGaAs quantum wells designed for polariton lasing

We report a systematic study of the temperature and excitation density behavior of an AlAs/AlGaAs, vertically emitting microcavity with embedded ternary Al0.20Ga0.80As/AlAs quantum wells in the strong coupling regime. Temperature-dependent photoluminescence measurements of the bare quantum wells indicate a crossover from the type-II indirect to the type-I direct transition. The resulting mixing of quantum well and barrier ground states in the conduction band leads to an estimated exciton binding energy systematically exceeding 25 meV. The formation of exciton-polaritons is evidenced in our quantum well microcavity via reflection measurements with Rabi splittings ranging from (13.93 ± 0.15) meV at low temperature (30 K) to (8.58 ± 0.40) meV at room temperature (300 K). Furthermore, the feasibility of polariton laser operation is demonstrated under non-resonant optical excitation conditions at 20 K and emission around 1.835 eV.

Exciton dynamics in solid-state green fluorescent protein

We study the decay characteristics of Frenkel excitons in solid-state enhanced green fluorescent protein (eGFP) dried from solution. We further monitor the changes of the radiative exciton decay over time by crossing the phase transition from the solved to the solid state. Complex interactions between protonated and deprotonated states in solid-state eGFP can be identified from temperature-dependent and time-resolved fluorescence experiments that further allow the determination of activation energies for each identified process.

Three-dimensional photonic confinement in imprinted liquid crystalline pillar microcavities

We demonstrate the feasibility of a thermal imprint technology capable of structuring organic thin films with liquid crystalline properties forming feature sizes on a several micrometer scale. The imprint technique can directly be applied onto a variety of substrates including dielectric mirrors. The so fabricated three-dimensional microcavities have lateral extensions up to 20u2009μm and heights between 1 and 5u2009μm. Exemplarily, pillar microcavities were produced wherein three-dimensional photonic confinement is observed by the formation of 0D cavity mode patterns. The imprint technique further favors the formation of hemispherical pillar geometries rather than cylindrical pillars, resulting in equidistant mode spacings of transversal cavity modes.

Polariton-lasing in microcavities filled with fluorescent proteins

Strong coupling between excitons and photons inside a microcavity leads to the formation of cavity polaritons, hybrid light-matter particles. Under suitable conditions, polaritons can emit coherent light without population inversion, whereby polariton lasing can exhibit a threshold at least an order of magnitude less than that of conventional photon lasing in the same material. Polaritons in organic semiconductors are stable at room temperature, due to their large exciton binding energy. This renders organic materials interesting for light-mater interaction experiments at ambient conditions. In this paper, we report on polariton-lasing using fluorescent proteins embedded in a planar microcavity. The typical laser-like threshold-behavior, manifesting in an intensity nonlinearity, coherence build-up with a linewidth drop and an interactioninduced blueshift stemming from the part-matter nature of polaritons are presented. Additionally, we show the possibility to confine photonic modes inside deterministically created traps by presenting discretized mode spectra.