An optical nanocavity incorporating a fluorescent organic dye having a high quality factor

We have fabricated an L3 optical nanocavity operating at visible wavelengths that is coated with a thin-film of a fluorescent molecular-dye. The cavity was directly fabricated into a pre-etched, free-standing silicon-nitride (SIN) membrane and had a quality factor of Q = 2650. This relatively high Q-factor approaches the theoretical limit that can be expected from an L3 nanocavity using silicon nitride as a dielectric material and is achieved as a result of the solvent-free cavity-fabrication protocol that we have developed. We show that the fluorescence from a red-emitting fluorescent dye coated onto the cavity surface undergoes strong emission intensity enhancement at a series of discrete wavelengths corresponding to the cavity modes. Three dimensional finite difference time domain (FDTD) calculations are used to predict the mode structure of the cavities with excellent agreement demonstrated between theory and experiment

Optical nanolithography using a scanning near-field probe with an integrated light source

An ultracompact near-field optical probe is described that is based on a single, integrated assembly consisting of a gallium nitride (GaN) light-emitting diode (LED), a microlens, and a cantilever assembly containing a hollow pyramidal probe with a subwavelength aperture at its apex. The LED emits ultraviolet light and may be used as a light source for near-field photolithographic exposure. Using this simple device compatible with many commercial atomic force microscope systems, it is possible to form nanostructures in photoresist with a resolution of 35 nm, corresponding to λ/10. © 2008 American Institute of Physics

A chemical sensor based on a photonic-crystal L3 nanocavity defined in a silicon-nitride membrane

The application of a silicon-nitride based L3 optical nanocavity as a chemical sensor is explored. It is shown that by adjusting the thickness of an ultra-thin Lumogen Red film deposited onto the nanocavity surface, the fundamental optical mode undergoes a progressive red-shift as the layer-thickness increases, with the cavity being able to detect the presence of a single molecular monolayer. The optical properties of a nanocavity whose surface is coated with a thin layer of a porphyrin-based polymer are also explored. On exposure of the cavity to an acidic-vapour, it is shown that changes in the optical properties of the porphyrin-film (thickness and refractive index) can be detected through a reversible shift in the cavity mode wavelength. Such effects are described using a finite difference time-domain model

Shaping potential landscape for organic polariton condensates in double-dye cavities

We investigate active spatial control of polariton condensates independently of the polariton-, gain-inducing excitation profile. This is achieved by introducing an extra intracavity semiconductor layer, non-resonant to the cavity mode. Saturation of the optical absorption in the uncoupled layer enables the ultra-fast modulation of the effective refractive index and, through excited-state absorption, the polariton dissipation. Utilising these mechanisms, we demonstrate control over the spatial profile and density of a polariton condensate at room temperature

Strong coupling in a microcavity containing β-carotene

© 2018 Optical Society of America. Abstract: We have fabricated an open-cavity microcavity structure containing a thin film of the biologically-derived molecule β-carotene. We show that the β-carotene absorption can be described in terms of a series of Lorentzian functions that approximate the 0-0, 0-1, 0-2, 0-3 and 0-4 electronic and vibronic transitions. On placing this molecular material into a microcavity, we obtain anti-crossing between the cavity mode and the 0-1 vibronic transition, however other electronic and vibronic transitions remain in the intermediate or weak-coupling regime due to their lower oscillator strength and broader linewidth. We discuss the consequences of strong-coupling for the possible modification of photosynthetic processes, or a re-ordering of allowed and optically-forbidden states

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

Nonlinear interactions of dipolar excitons and polaritons in MoS2 bilayers

Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons(dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit about 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This gives rise to a highly nonlinear regime which we describe theoretically by introducing a concept of hole crowding. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations

Molecular weight dependent vertical composition profiles of PCDTBT:PC71BM blends for organic photovoltaics

We have used Soxhlet solvent purification to fractionate a broad molecular weight distribution of the polycarbazole polymer PCDTBT into three lower polydispersity molecular weight fractions. Organic photovoltaic devices were made using a blend of the fullerene acceptor PC71BM with the molecular weight fractions. An average power conversion efficiency of 5.89% (peak efficiency of 6.15%) was measured for PCDTBT blend devices with a number average molecular weight of Mn = 25.5 kDa. There was significant variation between the molecular weight fractions with low (Mn = 15.0 kDa) and high (Mn = 34.9 kDa) fractions producing devices with average efficiencies of 5.02% and 3.70% respectively. Neutron reflectivity measurements on these polymer:PC71BM blend layers showed that larger molecular weights leads to an increase in the polymer enrichment layer thickness at the anode interface, this improves efficiency up to a limiting point where the polymer solubility causes a reduction of the PCDTBT concentration in the active layer

Binary solvent system used to fabricate fully annealing-free perovskite solar cells

High temperature post-deposition annealing of hybrid lead halide perovskite thin films—typically lasting at least 10 min—dramatically limits the maximum roll-to-roll coating speed, which determines solar module manufacturing costs. While several approaches for “annealing-free” perovskite solar cells (PSCs) have been demonstrated, many are of limited feasibility for scalable fabrication. Here, this work has solvent-engineered a high vapor pressure solvent mixture of 2-methoxy ethanol and tetrahydrofuran to deposit highly crystalline perovskite thin-films at room temperature using gas-quenching to remove the volatile solvents. Using this approach, this work demonstrates p-i-n devices with an annealing-free MAPbI3 perovskite layer achieving stabilized power conversion efficiencies (PCEs) of up to 18.0%, compared to 18.4% for devices containing an annealed perovskite layer. This work then explores the deposition of self-assembled molecules as the hole-transporting layer without annealing. This work finally combines the methods to create fully annealing-free devices having stabilized PCEs of up to 17.1%. This represents the state-of-the-art for annealing-free fabrication of PSCs with a process fully compatible with roll-to-roll manufacture