arXiv subjects

Rupert F. Oulton

Publications and source records attributed to Rupert F. Oulton.

30 records · Page 2Linked to original sources

arXiv2022

Near unity Raman $β$-factor of surface enhanced Raman scattering in a waveguide

The Raman scattering of light by molecular vibrations offers a powerful technique to 'fingerprint' molecules via their internal bonds and symmetries. Since Raman scattering is weak, methods to enhance, direct and harness it are highly desirable, e.g. through the use of optical cavities, waveguides, and surface enhanced Raman scattering (SERS). While SERS offers dramatic enhancements by localizing light within vanishingly small 'hot-spots' in metallic nanostructures, these tiny interaction volumes are only sensitive to few molecules, yielding weak signals that are difficult to detect. Here, we show that SERS from 4-Aminothiophenol (4-ATP) molecules bonded to a plasmonic gap waveguide is directed into a single mode with >99% efficiency. Although sacrificing a confinement dimension, we find 10$^4$ times SERS enhancement across a broad spectral range enabled by the waveguide's larger sensing volume and non-resonant mode. Remarkably, the waveguide-SERS (W-SERS) is bright enough to image Raman transport across the waveguides exposing the roles of nanofocusing and the Purcell effect. Emulating the $β$-factor from laser physics, the near unity Raman $β$-factor observed exposes the SERS technique in a new light and points to alternative routes to controlling Raman scattering. The ability of W-SERS to direct Raman scattering is relevant to Raman sensors based on integrated photonics with applications in gas and bio-sensing as well as healthcare.

physics.optics↗

arXiv2022

Solid immersion metalens for directional single molecule emission with high collection efficiency

We present simulations of an efficient high numerical aperture solid immersion metalens concept for fluorescence microscopy. The technique exploits the preferential emission of interfacial dipoles into a high refractive index substrate combined with a metalens and a conventional tube lens for imaging them. We have thus simulated dipole emission and an all-dielectric metasurface on opposite sides of a high refractive index substrate. Our calculations predict dipole collection efficiencies of up to 87 percent. The simulated beam propagation through the imaging system shows excellent performance along the optical axis, with aberrations accumulating with increasing field of view. These aberrations can be controlled by using a metasurface with an optimized non-hyperbolic phase profile. The high collection efficiency of dipole emission suggests this compact solid immersion lens would be effective for fluorescence imaging including single fluorescent centres for quantum optical application.

physics.optics↗

arXiv2021

Learning the Fuzzy Phases of Small Photonic Condensates

Phase transitions, being the ultimate manifestation of collective behaviour, are typically features of many-particle systems only. Here, we describe the experimental observation of collective behaviour in small photonic condensates made up of only a few photons. Moreover, a wide range of both equilibrium and non-equilibrium regimes, including Bose-Einstein condensation or laser-like emission are identified. However, the small photon number and the presence of large relative fluctuations places major difficulties in identifying different phases and phase transitions. We overcome this limitation by employing unsupervised learning and fuzzy clustering algorithms to systematically construct the fuzzy phase diagram of our small photonic condensate. Our results thus demonstrate the rich and complex phase structure of even small collections of photons, making them an ideal platform to investigate equilibrium and non-equilibrium physics at the few particle level.

cond-mat.quant-gas↗

arXiv2020

Transport and localization of light inside a dye-filled microcavity

The driven-dissipative nature of light-matter interaction inside a multimode, dye-filled microcavity makes it an ideal system to study nonequilibrium phenomena, such as transport. In this work, we investigate how light is efficiently transported inside such a microcavity, mediated by incoherent absorption and emission processes. In particular, we show that there exist two distinct regimes of transport, viz. conductive and localized, arising from the complex interplay between the thermalizing effect of the dye molecules and the nonequilibrium influence of driving and loss. The propagation of light in the conductive regime occurs when several localized cavity modes undergo dynamical phase transitions to a condensed, or lasing, state. Further, we observe that while such transport is robust for weak disorder in the cavity potential, strong disorder can lead to localization of light even under good thermalizing conditions. Importantly, the exhibited transport and localization of light is a manifestation of the nonequilibrium dynamics rather than any coherent interference in the system.

quant-ph↗

arXiv2020

Plasmon-Driven Hot Electron Transfer at Atomically Sharp Metal-Semiconductor Nanojunctions

Recent advances in guiding and localizing light at the nanoscale exposed the enormous potential of ultra-scaled plasmonic devices. In this context, the decay of surface plasmons to hot carriers triggers a variety of applications in boosting the efficiency of energy-harvesting, photo-catalysis and photo-detection. However, a detailed understanding of plasmonic hot carrier generation and particularly the transfer at metal-semiconductor interfaces is still elusive. In this paper, we introduce a monolithic metal-semiconductor (Al-Ge) heterostructure device, providing a platform to examine surface plasmon decay and hot electron transfer at an atomically sharp Schottky nanojunction. The gated metal-semiconductor heterojunction device features electrostatic control of the Schottky barrier height at the Al-Ge interface, enabling hot electron filtering. The ability of momentum matching and to control the energy distribution of plasmon-driven hot electron injection is demonstrated by controlling the interband electron transfer in Ge leading to negative differential resistance.

physics.app-ph↗

arXiv2019

Non-stationary Statistics and Formation Jitter in Transient Photon Condensation

While equilibrium phase transitions are well described by a free-energy landscape, there are few tools to describe general features of their non-equilibrium counterparts. On the other hand, near-equilibrium free-energies are easily accessible but their full geometry is only explored in non-equilibrium, e.g. after a quench. In the particular case of a non-stationary system, however, the concepts of an order parameter and free energy become ill-defined, and a comprehensive understanding of non-stationary (transient) phase transitions is still lacking. Here, we probe transient non-equilibrium dynamics of an optically pumped, dye-filled microcavity which exhibits near-equilibrium Bose-Einstein condensation under steady-state conditions. By rapidly exciting a large number of dye molecules, we quench the system to a far-from-equilibrium state and, close to a critical excitation energy, find delayed condensation, interpreted as a transient equivalent of critical slowing down. We introduce the two-time, non-stationary, second-order correlation function as a powerful experimental tool for probing the statistical properties of the transient relaxation dynamics. In addition to number fluctuations near the critical excitation energy, we show that transient phase transitions exhibit a different form of diverging fluctuations, namely timing jitter in the growth of the order parameter. This jitter is seeded by the randomness associated with spontaneous emission, with its effect being amplified near the critical point. The general character of our results are then discussed based on the geometry of effective free-energy landscapes. We thus identify universal features, such as the formation timing jitter, for a larger set of systems undergoing transient phase transitions. Our results carry immediate implications to diverse systems, including micro- and nano-lasers and growth of colloidal nanoparticles.

cond-mat.stat-mech↗

arXiv2019

Hybrid plasmonic waveguide coupling of photons from a single molecule

We demonstrate the emission of photons from a single molecule into a hybrid gap plasmon waveguide (HGPW). Crystals of anthracene, doped with dibenzoterrylene (DBT), are grown on top of the waveguides. We investigate a single DBT molecule coupled to the plasmonic region of one of the guides, and determine its in-plane orientation, excited state lifetime and saturation intensity. The molecule emits light into the guide, which is remotely out-coupled by a grating. The second-order auto-correlation and cross-correlation functions show that the emitter is a single molecule and that the light emerging from the grating comes from that molecule. The coupling efficiency is found to be $β_{WG}=11.6(1.5)\%$. This type of structure is promising for building new functionality into quantum-photonic circuits, where localised regions of strong emitter-guide coupling can be interconnected by low-loss dielectric guides.

quant-ph↗

arXiv2018

Optimizing hot electron harvesting at planar metal-semiconductor interfaces with titanium oxynitride thin films

Understanding metal-semiconductor interfaces is critical to the advancement of photocatalysis and sub-bandgap solar energy harvesting where sub-bandgap photons can be excited and extracted into the semiconductor. In this work, we compare the electron extraction efficiency across Au/TiO2 and titanium oxynitride/TiO2-x interfaces, where in the latter case the spontaneously forming oxide layer (TiO2-x) creates a metal-semiconductor contact. Time-resolved pump-probe spectroscopy is used to study the electron recombination rates in both cases. Unlike the nanosecond recombination lifetimes in Au/TiO2, we find a bottleneck in the electron relaxation in the TiON system, which we explain using a trap-mediated recombination model. Using this model, we investigate the tunability of the relaxation dynamics with oxygen content in the parent film. The optimized film (TiO0.5N0.5) exhibits the highest carrier extraction efficiency, slowest trapping and an appreciable hot electron population reaching the surface oxide. Our results demonstrate the productive role oxygen can play in enhancing electron harvesting and elongating electron lifetimes providing an optimized metal-semiconductor interface using only the native oxide of titanium oxynitride.

cond-mat.mes-hall↗

arXiv2017

Efficient four-wave mixing at the nanofocus of integrated organic gap plasmon waveguides on silicon

Nonlinear optics, especially frequency mixing, underpins modern optical technology and scientific exploration in quantum optics, materials and life sciences, and optical communications. Since nonlinear effects are weak, efficient frequency mixing must accumulate over large interaction lengths restricting the integration of nonlinear photonics with electronics and establishing limitations on mixing processes due to the requirement of phase matching. In this work we report efficient four-wave mixing over micron-scale interaction lengths at telecoms wavelengths. We use an integrated plasmonic gap waveguide on silicon that strongly confines light within a nonlinear organic polymer in the gap. Our approach is so effective because the gap waveguide intensifies light by efficiently nanofocusing it to a mode cross-section of a few tens of nanometres, generating a nonlinear response so strong that efficient four-wave mixing accumulates in just a micron. This is significant as our technique opens up nonlinear optics to a regime where phase matching and dispersion considerations are relaxed, giving rise to the possibility of compact, broadband, and efficient frequency mixing on a platform that can be integrated with silicon photonics.

physics.optics↗

arXiv2017

Titanium oxynitride thin films with tunable double epsilon-near-zero behaviour

Titanium Oxynitride (TiOxNy) thin films are fabricated using reactive magnetron sputtering. The mechanism of their growth formation is explained and their optical properties are presented. The films grown when the level of residual Oxygen in the background vacuum was between 5E-9Torr to 20E-9Torr exhibit double Epsilon-Near-Zero (2-ENZ) behaviour with ENZ1 and ENZ2 wavelengths tunable in the 700-850 nm and in the 1100-1350 nm spectral ranges, respectively. Samples fabricated when the level of residual Oxygen in the background vacuum was above 2E-8Torr exhibit non-metallic behaviour, while the layers deposited when the level of residual Oxygen in the background vacuum was below 5E-9Torr, show metallic behaviour with a single ENZ value. The double ENZ phenomenon is related to the level of residual Oxygen in the background vacuum and is attributed to the mixture of TiN and TiOxNy/TiOx phases in the films. Varying the partial pressure of nitrogen during the deposition can further control the amount of TiN, TiOx and TiOxNy compounds in the films and, therefore, tune the screened plasma wavelength. A good approximation of the ellipsometric behaviour is achieved with Maxwell-Garnett theory for a composite film formed by a mixture of TiO2 and TiN phases suggesting that double ENZ TiOxNy films are formed by inclusions of TiN within a TiO2 matrix. These oxynitride compounds could be considered as new materials exhibiting double ENZ in the visible and near-IR spectral ranges.

cond-mat.mtrl-sci↗

arXiv2015

Measuring chromatic aberrations in imaging systems using plasmonic nano-particles

Chromatic aberration in optical systems arises from the wavelength dependence of a glass's refractive index. Polychromatic rays incident upon an optical surface are refracted at slightly different angles and in traversing an optical system follow distinct paths creating images displaced according to color. Although arising from dispersion, it manifests as a spatial distortion correctable only with compound lenses with multiple glasses and accumulates in complicated imaging systems. While chromatic aberration is measured with interferometry, simple methods are attractive for their ease of use and low cost. In this letter we retrieve the longitudinal chromatic focal shift of high numerical aperture (NA) microscope objectives from the extinction spectra of metallic nanoparticles within the focal plane. The method is accurate for high NA objectives with apochromatic correction, and enables rapid assessment of the chromatic aberration of any complete microscopy systems, since it is straightforward to implement

physics.optics↗

arXiv2015

Geometric interpretations for resonances of plasmonic nanoparticles

The rapidly developing field of plasmonics can be roughly categorized into two branches: surface plasmon polaritons (SPPs) propagating in plasmonic waveguides and localized surface plasmons (LSPs) supported by scattering plasmonic particles. Investigations along these two directions usually employ quite different approaches and techniques, resulting in more or less a dogma that the two branches progress almost independently of each other, with few interactions. Here in this work we interpret LSPs from a Bohr model based geometric perspective relying on SPPs, thus establishing a connection between these two sub-fields. Besides the clear explanations of conventional scattering features of plasmonic nanoparticles, based on this geometric model we further demonstrate other anomalous scattering features (higher order modes supported at lower frequencies, and blueshift of the resonance with increasing particle sizes) and multiple electric resonances of the same order supported at different frequencies, which have been revealed to originate from backward SPP modes and multiple dispersion bands supported in the corresponding plasmonic waveguides, respectively. Inspired by this geometric model, it is also shown that, through solely geometric tuning, the absorption of each LSP resonance can be maximized to reach the single channel absorption limit, provided that the scattering and absorption rates are tuned to be equal. The Bohr model based geometric picture offers new insights into the understanding of the localized resonances, and may shed new light to many related applications based on particle scattering, such as biosensing, nanoantennas, photovoltaic devices and related medical treatment.

physics.optics↗