Controlling the Spatial Profile and Energy Landscape of Organic Polariton Condensates in Double-Dye Cavities.

The development of high-speed, all-optical polariton logic devices underlies emerging unconventional computing technologies and relies on advancing techniques to reversibly manipulate the spatial extent and energy of polartion condensates. We investigate active spatial control of polariton condensates independent of the polariton, gain-inducing excitation profile. This is achieved by introducing an extra intracavity semiconductor layer, nonresonant to the cavity mode. Partial saturation of the optical absorption in the uncoupled layer enables the ultrafast modulation of the effective refractive index and, through excited-state absorption, the polariton dissipation. Utilizing an intricate interplay of these mechanisms, we demonstrate control over the spatial profile, density, and energy of a polariton condensate at room temperature.

k-Space Hyperspectral Imaging by a Birefringent Common-Path Interferometer.

Fourier-plane microscopy is a powerful tool for measuring the angular optical response of a plethora of materials and photonic devices. Among them, optical microcavities feature distinctive energy-momentum dispersions, crucial for a broad range of fundamental studies and applications. However, measuring the whole momentum space (k-space) with sufficient spectral resolution using standard spectroscopic techniques is challenging, requiring long and alignment-sensitive scans. Here, we introduce a k-space hyperspectral microscope, which uses a common-path birefringent interferometer to image photoluminescent organic microcavities, obtaining an angle- and wavelength-resolved view of the samples in only one measurement. The exceptional combination of angular and spectral resolution of our technique allows us to reconstruct a three-dimensional (3D) map of the cavity dispersion in the energy-momentum space, revealing the polarization-dependent behavior of the resonant cavity modes. Furthermore, we apply our technique for the characterization of a dielectric nanodisk metasurface, evidencing the angular and spectral behavior of its anapole mode. This approach is able to provide a complete optical characterization for materials and devices with nontrivial angle-/wavelength-dependent properties, fundamental for future developments in the fields of topological photonics and optical metamaterials.

Dephasing Processes in the Molecular Dye Lumogen-F Orange Characterized by Two-Dimensional Electronic Spectroscopy.

Molecular dyes are finding more and more applications in photonics and quantum technologies, such as polaritonic optical microcavities, organic quantum batteries and single-photon emitters for quantum sensing and metrology. For all these applications, it is of crucial importance to characterize the dephasing mechanisms. In this work we use two-dimensional electronic spectroscopy (2DES) to study the temperature dependent dephasing processes in the prototypical organic dye Lumogen-F orange. We model the 2DES maps using the Bloch equations for a two-level system and obtain a dephasing time T2 = 53 fs at room temperature, which increases to T2 = 94 fs at 86 K. Furthermore, spectral diffusion processes are observed and modeled by a combination of underdamped and overdamped Brownian oscillators. Our results provide useful design parameters for advanced optoelectronic and photonic devices incorporating dye molecules.

Superabsorption in an organic microcavity: Toward a quantum battery.

The rate at which matter emits or absorbs light can be modified by its environment, as markedly exemplified by the widely studied phenomenon of superradiance. The reverse process, superabsorption, is harder to demonstrate because of the challenges of probing ultrafast processes and has only been seen for small numbers of atoms. Its central idea­superextensive scaling of absorption, meaning larger systems absorb faster­is also the key idea underpinning quantum batteries. Here, we implement experimentally a paradigmatic model of a quantum battery, constructed of a microcavity enclosing a molecular dye. Ultrafast optical spectroscopy allows us to observe charging dynamics at femtosecond resolution to demonstrate superextensive charging rates and storage capacity, in agreement with our theoretical modeling. We find that decoherence plays an important role in stabilizing energy storage. Our work opens future opportunities for harnessing collective effects in light-matter coupling for nanoscale energy capture, storage, and transport technologies.

Polariton condensation in an organic microcavity utilising a hybrid metal-DBR mirror.

We have developed a simplified approach to fabricate high-reflectivity mirrors suitable for applications in a strongly-coupled organic-semiconductor microcavity. Such mirrors are based on a small number of quarter-wave dielectric pairs deposited on top of a thick silver film that combine high reflectivity and broad reflectivity bandwidth. Using this approach, we construct a microcavity containing the molecular dye BODIPY-Br in which the bottom cavity mirror is composed of a silver layer coated by a SiO2 and a Nb2O5 film, and show that this cavity undergoes polariton condensation at a similar threshold to that of a control cavity whose bottom mirror consists of ten quarter-wave dielectric pairs. We observe, however, that the roughness of the hybrid mirror-caused by limited adhesion between the silver and the dielectric pair-apparently prevents complete collapse of the population to the ground polariton state above the condensation threshold.

Observation of photon-mode decoupling in a strongly coupled multimode microcavity.

We have fabricated organic semiconductor microcavities having an extended optical path-length (up to 2 µm) that contain J-aggregates of a cyanine dye. These structures are studied using optical-reflectivity and are found to be characterized by a series of polaritonic modes. By changing the effective oscillator strength of the dye within the cavity, we evidence a transition from "normal" strong coupling in which the photon modes are coupled to one another via the excitonic transition of the molecular dye to a state in which photon-modes become decoupled. We use an eight-level modified Hamiltonian to describe the optical properties of the system and compare the distribution of the confined optical field in coupled and decoupled structures.