arXiv subjects

William L. Barnes

Publications and source records attributed to William L. Barnes.

At least 19 recordsLinked to original sources

arXiv2026

Nanoparticle Arrays for Efficient Organic Light-Emitting Diode Emission Management

OLEDs are increasingly applied in illumination and displays because they offer excellent color quality, are mechanically flexible, and are self-emissive. However, their usage is limited by low external quantum efficiency (EQE) and efficiency roll-off at high driving voltages. These limitations, together with demands for smaller pixels and device sizes in emerging technologies, motivate innovations that increase efficiency and allow replacing external optical elements with embedded solutions. Here, we demonstrate enhanced outcoupling as well as directional and polarization control of OLED emission, based on collective surface lattice resonances of plasmonic nanoparticle arrays that are embedded in the active layers of four different state-of-the-art OLED structures. Both square arrays and more complex lattices producing flat bands are demonstrated to guide the light to directions and polarizations determined by their optical modes. We show that by the design of the array geometry and the OLED structure, spectral and angular enhancement of the electroluminescence (EL), up to 30 %, can be achieved. Our results verify that surface lattice resonances of nanoparticle arrays offer a robust and versatile embedded solution for tailoring the OLED emission, as well as exciting prospects for efficiency increase if combined with narrow-spectrum emitters.

physics.optics↗

arXiv2025

Generating phase singularities using surface exciton polaritons in an organic natural hyperbolic material

Surface polaritons (SPs) are electromagnetic waves bound to a surface through their interaction with charge carriers in the surface material. Hyperbolic SPs can be supported by optically anisotropic materials where the in-plane and out-of-plane permittivies have opposite signs. Here we report what we believe to be the first experimental study of hyperbolic surface exciton polaritons (HSEPs). We study the intensity and phase response of HSEPs in the J-aggregate TDBC (a type-II natural hyperbolic material). HSEPs can be used to generate phase singularities; the behaviour of these phase singularities is a consequence of the hyperbolic nature of TDBC. The combined intensity and phase response of non-hyperbolic and hyperbolic SPs suggests that they are topologically distinct. We predict analogous effects for hyperbolic surface phonon polaritons in hexagonal boron nitride. Our work suggests that organic materials can provide a new platform for the exploration of hyperbolic surface polaritonics at visible frequencies.

cond-mat.mes-hall↗

arXiv2025

Response to Comment on "Non-Polaritonic Effects in Cavity-Modified Photochemistry": On the Importance of Experimental Details

This note responds to Schwartz and Hutchison's Comment (arXiv:2403.06001) on our article (DOI:10.1002/adma.202309393). We think differences have arisen not in the experimental results themselves but in their interpretation: our more extensive experiments allowed us to distinguish between "true positive" and "false positive" results. We identify potential evidence of non-polaritonic effects in Schwartz and Hutchison's own work. We hope our work will encourage others to produce more systematic investigations of strong coupling.

physics.chem-ph↗

arXiv2025

Dispersion of backward-propagating waves in a surface defect on a 3D photonic band gap crystal

We experimentally study the dispersion relation of waves in a two-dimensional (2D) defect layer with periodic nanopores that sits on a three-dimensional (3D) photonic band gap crystal made from silicon by CMOS-compatible methods. The nanostructures are probed by momentum-resolved broadband near-infrared imaging of p-polarized reflected light that is collected inside the light cone as a function of off-axis wave vectors. We identify surface defect modes at frequencies inside the band gap with a narrow relative linewidth ($Δω/ω$ = 0.028), which are absent in defect-free 3D crystals. We calculate the dispersion of modes with relevant mode symmetries using a plane-wave-expansion supercell method with no free parameters. The calculated dispersion matches very well with the measured data. The dispersion is negative in one of the off-axis directions, corresponding to backward-propagating waves where the phase velocity and the group velocity point in opposite directions, as confirmed by finite-difference time-domain simulations. We also present an analytic model of a 2D grating sandwiched between vacuum and a negative real $ε'$ < 0 that mimics the 3D photonic band gap. The model's dispersion agrees with the experiments and with the fuller theory and shows that the backward propagation is caused by the surface grating. We discuss possible applications, including a device that senses the output direction of photons emitted by quantum emitters in response to their frequency.

physics.optics↗

arXiv2024

Molecular Strong Coupling and Cavity Finesse

Molecular strong coupling offers exciting prospects in physics, chemistry and materials science. Whilst attention has been focused on developing realistic models for the molecular systems, the important role played by the entire photonic mode structure of the optical cavities has been less explored. We show that the effectiveness of molecular strong coupling may be critically dependent on cavity finesse. Specifically we only see emission associated with a dispersive lower polariton for cavities with sufficient finesse. By developing an analytical model of cavity photoluminescence in a multimode structure we clarify the role of finite-finesse in polariton formation, and show that lowering the finesse reduces the extent of the mixing of light and matter in polariton states. We suggest that the detailed nature of the photonic modes supported by a cavity will be as important in developing a coherent framework for molecular strong coupling as the inclusion of realistic molecular models.

physics.optics↗

arXiv2024

Multiple Interacting Photonic Modes in Strongly Coupled Organic Microcavities

Room temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of a vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low finesse multi-mode situations we find that molecular dipoles can be partially hybridised with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.

quant-ph↗

arXiv2024

Long-range molecular energy transfer mediated by strong coupling to plasmonic topological edge states

Strong coupling between light and molecular matter is currently attracting interest both in chemistry and physics, in the fast-growing field of molecular polaritonics. The large near-field enhancement of the electric field of plasmonic surfaces and their high tunability make arrays of metallic nanoparticles an interesting platform to achieve and control strong coupling. Two dimensional plasmonic arrays with several nanoparticles per unit cell and crystalline symmetries can host topological edge and corner states. Here we explore the coupling of molecular materials to these edge states using a coupled-dipole framework including long-range interactions. We study both the weak and strong coupling regimes and demonstrate that coupling to topological edge states can be employed to enhance highly-directional long-range energy transfer between molecules.

cond-mat.mes-hall↗

arXiv2024

Strong coupling in molecular systems: a simple predictor employing routine optical measurements

We provide a simple method that enables readily acquired experimental data to be used to predict whether or not a candidate molecular material may exhibit strong coupling. Specifically, we explore the relationship between the hybrid molecular/photonic (polaritonic) states and the bulk optical response of the molecular material. For a given material this approach enables a prediction of the maximum extent of strong coupling (vacuum Rabi splitting), irrespective of the nature of the confined light field. We provide formulae for the upper limit of the splitting in terms of the molar absorption coefficient, the attenuation coefficient, the extinction coefficient (imaginary part of the refractive index) and the absorbance. To illustrate this approach we provide a number of examples, we also discuss some of the limitations of our approach.

physics.optics↗

arXiv2023

Non-polaritonic effects in cavity-modified photochemistry

Strong coupling of molecules to vacuum fields has been widely reported to lead to modified chemical properties such as reaction rates. However, some recent attempts to reproduce infrared strong coupling results have not been successful, suggesting that factors other than strong coupling may sometimes be involved. Here we re-examine the first of these vacuum-modified chemistry experiments in which changes to a molecular photoisomerisation process in the UV-vis spectral range were attributed to strong coupling of the molecules to visible light. We observed significant variations in photoisomerisation rates consistent with the original work; however, we found no evidence that these changes need to be attributed to strong coupling. Instead, we suggest that the photoisomerisation rates involved are most strongly influenced by the absorption of ultraviolet radiation in the cavity. Our results indicate that care must be taken to rule out non-polaritonic effects before invoking strong coupling to explain any changes of chemical properties arising in cavity-based experiments.

cond-mat.mes-hall↗

arXiv2023

Raman-probing the local ultrastrong coupling of vibrational plasmon-polaritons on metallic gratings

Strong coupling of molecular vibrations with light creates polariton states, enabling control over many optical and chemical properties. However, the near-field signatures of strong coupling are difficult to map as most cavities are closed systems. Surface-enhanced Raman microscopy of open metallic gratings under vibrational strong coupling enables the observation of spatial polariton localization in the grating near-field, without the need for scanning probe microscopies. The lower polariton is localized at the grating slots, displays a strongly asymmetric lineshape, and gives greater plasmon-vibration coupling strength than measured in the far-field. Within these slots, the local field strength pushes the system into the ultrastrong coupling regime. Models of strong coupling which explicitly include the spatial distribution of emitters can account for these effects. Such gratings form a new system for exploring the rich physics of polaritons and the interplay between their near- and far-field properties through polariton-enhanced Raman scattering (PERS).

physics.optics↗

arXiv2021

All-optical control of phase singularities using strong light-matter coupling

Strong light-matter coupling occurs when the coupling strength between a confined electromagnetic mode and a molecular resonance exceeds losses to the environment. The study of strong coupling has been motivated by applications such as lasing and the modification of chemical processes. Here we show that strong coupling can be used to create phase singularities. Many nanophotonic structures have been designed to generate phase singularities for use in sensing and optoelectronics. We utilise the concept of cavity-free strong coupling, where electromagnetic modes sustained by a material are strong enough to strongly couple to the material's own molecular resonance, to create phase singularities in a simple thin film of organic molecules. We show that the use of photochromic molecules allows for all-optical control of phase singularities. Our results suggest a new application for strong light-matter coupling and a new, simplified, more versatile pathway to singular phase optics.

cond-mat.mes-hall↗

arXiv2021

Wavefront shaping to improve beam quality: converting a speckle pattern into a Gaussian spot

A perfectly collimated beam can be spread out by multiple scattering, creating a speckle pattern and increasing the etendue of the system. Standard optical systems conserve etendue, and thus are unable to reverse the process by transforming a speckle pattern into a collimated beam or, equivalently, into a sharp focus. Wavefront shaping is a technique that is able to manipulate the amplitude and/or phase of a light beam, thus controlling its propagation through such media. Wavefront shaping can thus break the conservation of etendue and, in principle, reduce it. In this work we study how much of the energy contained in a fully developed speckle pattern can be converted into a high quality (low M2) beam, and discuss the advantages and limitations of this approach, with special attention given to the inherent variability in the quality of the output due to the multiple scattering.

physics.optics↗

arXiv2020

A new signature for strong light-matter coupling using spectroscopic ellipsometry

Light-matter interactions can occur when an ensemble of molecular resonators is placed in a confined electromagnetic field. In the strong coupling regime the rapid exchange of energy between the molecules and the electromagnetic field results in the emergence of hybrid light-matter states called polaritons. Multiple criteria exist to define the strong coupling regime, usually by comparing the splitting of the polariton bands with the linewidths of the uncoupled modes. Here we highlight the limitations of these criteria and study strong coupling using spectroscopic ellipsometry, a commonly used optical characterisation technique. We identify a new signature of strong coupling in ellipsometric phase spectra. Combining ellipsometric amplitude and phase spectra yields a distinct topological feature that we suggest could serve as a new criterion for strong coupling. Our results introduce the idea of ellipsometric topology and could provide further insight into the transition from the weak to strong coupling regime.

cond-mat.mes-hall↗

arXiv2019

Electrically tuneable exciton energy exchange between spatially separated 2-dimensional semiconductors in a microcavity

Electrical control over the energy exchange between exciton states mediated by cavity-polaritons at room temperature is demonstrated. Spatially separated field effect transistors based on monolayers of WS$_2$ and MoS$_2$ are placed in a tuneable Fabry-Pérot microcavity. This device is specially designed for the formation of exciton-polaritons that combine the two exciton species and a tuneable cavity mode. It is further shown that the tuning of the free carrier density in the WS$_2$ film leads to a strong modulation of the Rabi splitting that modifies the excitonic and photonic nature of exciton-polaritons. Electrical control of polaritonic devices may lead to technological applications using switchable quantum states.

cond-mat.mes-hall↗

arXiv2019

Electrically tuneable exciton-polaritons through free electron doping in monolayer WS$_2$ microcavities

We demonstrate control over light-matter coupling at room temperature combining a field effect transistor (FET) with a tuneable optical microcavity. Our microcavity FET comprises a monolayer tungsten disulfide WS$_2$ semiconductor which was transferred onto a hexagonal boron nitride flake that acts as a dielectric spacer in the microcavity, and as an electric insulator in the FET. In our tuneable system, strong coupling between excitons in the monolayer WS$_2$ and cavity photons can be tuned by controlling the cavity length, which we achieved with excellent stability, allowing us to choose from the second to the fifth order of the cavity modes. Once we achieve the strong coupling regime, we then modify the oscillator strength of excitons in the semiconductor material by modifying the free electron carrier density in the conduction band of the WS$_2$. This enables strong Coulomb repulsion between free electrons, which reduces the oscillator strength of excitons until the Rabi splitting completely disappears. We controlled the charge carrier density from 0 up to 3.2 $\times$ 10$^{12}$ cm$^{-2}$, and over this range the Rabi splitting varies from a maximum value that depends on the cavity mode chosen, down to zero, so the system spans the strong to weak coupling regimes.

cond-mat.mes-hall↗

arXiv2019

Strong Light-Matter Coupling in Carbon Nanotubes as a Route to Exciton Brightening

We show that strong light-matter coupling can be used to overcome a long standing problem that has prevented efficient optical emission from carbon nanotubes. The luminescence from the nominally bright exciton states of carbon nanotubes is quenched due to the fast nonradiative scattering to the dark exciton state having a lower energy. We present a theoretical analysis to show that by placing carbon nanotubes in an optical microcavity the bright exctonic state may be split into two hybrid exciton-polariton states, while the dark state remains unaltered. For sufficiently strong coupling between the bright exciton and the cavity, we show that the energy of the lower polariton may be pushed below that of the dark exciton. This overturning of the relative energies of the bright and dark excitons prevents the dark exciton from quenching the emission. Our resutls pave the way for a new approach to band-engineering the properties of the nanoscale optoelectronic devices.

cond-mat.mes-hall↗

arXiv2019

Nanoscale design of the local density of optical states

We propose a design concept for tailoring the local density of optical states (LDOS) in dielectric nanostructures, based on the phase distribution of the scattered optical fields induced by point-like emitters. First we demonstrate that the LDOS can be expressed in terms of a coherent summation of constructive and destructive contributions. By using an iterative approach, dielectric nanostructures can be designed to effectively remove the destructive terms. In this way dielectric Mie resonators, featuring low LDOS for electric dipoles, can be reshaped to enable enhancements of three orders of magnitude. To demonstrate the generality of the method, we also design nanocavities that enhance the radiated power of a circular dipole, a quadrupole and an arbitrary collection of coherent dipoles. Our concept provides a powerful tool for high-performance dielectric resonators, and affords fundamental insights into light-matter coupling at the nanoscale.

physics.optics↗

arXiv2018

Manipulating type-I and type-II Dirac polaritons in cavity-embedded honeycomb metasurfaces

Pseudorelativistic Dirac quasiparticles have emerged in a plethora of artificial graphene systems that mimic the underlying honeycomb symmetry of graphene. However, it is notoriously difficult to manipulate their properties without modifying the lattice structure. Here we theoretically investigate polaritons supported by honeycomb metasurfaces and, despite the trivial nature of the resonant elements, we unveil rich Dirac physics stemming from a non-trivial winding in the light-matter interaction. The metasurfaces simultaneously exhibit two distinct species of massless Dirac polaritons, namely type-I and type-II. By modifying only the photonic environment via an enclosing cavity, one can manipulate the location of the type-II Dirac points, leading to qualitatively different polariton phases. This enables one to alter the fundamental properties of the emergent Dirac polaritons while preserving the lattice structure - a unique scenario which has no analog in real or artificial graphene systems. Exploiting the photonic environment will thus give rise to unexplored Dirac physics at the subwavelength scale.

physics.optics↗