arXiv subjects

Robert A. Taylor

Publications and source records attributed to Robert A. Taylor.

14 recordsLinked to original sources

arXiv2026

Carrier Localization in Pnictogen-Based Chalcohalides from Defect-Bound Hot Polarons

Pnictogen-based solar absorbers have gained prominence as promising nontoxic and stable alternatives to lead-halide perovskites (LHPs), but are severely limited by carrier localization, preventing their performance from approaching those of LHPs. Recent efforts have uncovered routes to overcome carrier localization, but these early efforts only considered intrinsic factors. Herein, we push beyond these limited early efforts, examining the role of defects, not only on cold carriers but also hot carriers. Focusing on the structurally one-dimensional pnictogen chalcohalide BiSBr, we find that whilst this material intrinsically does not exhibit carrier localization, vacancies introduced during synthesis or post-treatment lead to pronounced extrinsic self-trapping via the formation of defect-bound hot polarons-excited charge-carriers strongly coupled to local defect-induced vibrational modes. These above-gap defect states divert hot carriers from cooling to the band edge, thus depleting the mobile carrier population. Our findings establish the key role of defect-bound hot polarons in mediating extrinsic localization and offer new mechanistic insights into the interplay between defects, lattice coupling, and excited-state charge-carrier transport, which are critical to designing efficient perovskite-inspired solar absorbers.

cond-mat.mtrl-sci↗

arXiv2023

Ultranarrow linewidth room-temperature single-photon source from perovskite quantum dot embedded in optical microcavity

Ultranarrow bandwidth single-photon sources operating at room-temperature are of vital importance for viable optical quantum technologies at scale, including quantum key distribution, cloud based quantum information processing networks, and quantum metrology. Here we show a room-temperature ultranarrow bandwidth single-photon source generating polarised photons at a rate of 5MHz based on an inorganic CsPbI3 perovskite quantum dot embedded in a tunable open-access optical microcavity. When coupled to an optical cavity mode, the quantum dot room-temperature emission becomes single-mode and the spectrum narrows down to just 1 nm. The low numerical aperture of the optical cavities enables efficient collection of high-purity single-mode single-photon emission at room-temperature, offering promising performance for photonic and quantum technology applications. We measure 94% pure single-photon emission into a single-mode under pulsed and continuous-wave (CW) excitation.

physics.optics↗

arXiv2023

Three-photon excitation of quantum two-level systems

We demonstrate that semiconductor quantum dots can be excited efficiently in a resonant three-photon process, whilst resonant two-photon excitation is highly suppressed. Time-dependent Floquet theory is used to quantify the strength of the multi-photon processes and model the experimental results. The efficiency of these transitions can be drawn directly from parity considerations in the electron and hole wavefunctions in semiconductor quantum dots. Finally, we exploit this technique to probe intrinsic properties of InGaN quantum dots. In contrast to non-resonant excitation, slow relaxation of charge carriers is avoided which allows us to measure directly the radiative lifetime of the lowest energy exciton states. Since the emission energy is detuned far from the resonant driving laser field, polarization filtering is not required and emission with a greater degree of linear polarization is observed compared to non-resonant excitation.

quant-ph↗

arXiv2022

Design of free-space couplers for suspended triangular nano-beam waveguides

Photonic waveguides with triangular cross section are being investigated for material systems such as diamond, glasses and gallium nitride, which lack easy options to create conventional rectangular nanophotonic waveguides. The design rules for optical elements in these triangular waveguides, such as couplers and gratings, are not well established. Here we present simulations of elements designed to couple light into, and out of, triangular waveguides from the vertical direction, which can be implemented with current angled-etch fabrication technology. The devices demonstrate coupling efficiencies approaching \unit{50}{\%} for light focused from a high numerical aperture objective. The implementation of such couplers will enable fast and efficient testing of closely spaced integrated circuit components.

physics.optics↗

arXiv2021

Resonantly pumped bright-triplet exciton lasing in caesium lead bromide perovskites

The surprising recent observation of highly emissive triplet-states in lead halide perovskites accounts for their orders-of-magnitude brighter optical signals and high quantum efficiencies compared to other semiconductors. This makes them attractive for future optoelectronic applications, especially in bright low-threshold nano-lasers. Whilst non-resonantly pumped lasing from all-inorganic lead-halide perovskites is now well-established as an attractive pathway to scalable low-power laser sources for nano-optoelectronics, here we showcase a resonant optical pumping scheme on a fast triplet-state in CsPbBr3 nanocrystals. The scheme allows us to realize a polarized triplet-laser source that dramatically enhances the coherent signal by one order of magnitude whilst suppressing non-coherent contributions. The result is a source with highly attractive technological characteristics including a bright and polarized signal, and a high stimulated-to-spontaneous emission signal contrast that can be filtered to enhance spectral purity. The emission is generated by pumping selectively on a weakly-confined excitonic state with a Bohr radius ~10 nm in the nanocrystals. The exciton fine-structure is revealed by the energy-splitting resulting from confinement in nanocrystals with tetragonal symmetry. We use a linear polarizer to resolve two-fold non-degenerate sub-levels in the triplet exciton and use photoluminescence excitation spectroscopy to determine the energy of the state before pumping it resonantly.

physics.optics↗

arXiv2019

Reduction of radiative lifetime and slow-timescale spectral diffusion in InGaN polarized single-photon sources

Non-polar (11-20) a-plane quantum dots (QDs) are strong candidates for both > 200 K on-chip ultrafast polarized single-photon generation and the investigation of high temperature semiconductor QD photophysics. In this work, we report progress in the growth of a-plane InGaN QDs with a quasi-two-temperature method, which produces smooth epilayers and significantly reduced carrier trapping sites in the proximity of the QDs. Optical characterization has confirmed the ability of such QDs to emit polarized single photons and we have recorded a ~ 45% shorter average radiative lifetime and 65% reduction in the slow-timescale spectral diffusion compared to previous QDs. This growth method is an important development of the non-polar a-plane InGaN platform, opening up more possibilities in single-photon, lasing, and fundamental investigations.

cond-mat.mes-hall↗

arXiv2017

Electrically tunable organic-inorganic hybrid polaritons with monolayer WS2

Exciton-polaritons are quasiparticles consisting of a linear superposition of photonic and excitonic states, offering potential for nonlinear optical devices. The excitonic component of the polariton provides a finite Coulomb scattering cross section, such that the different types of exciton found in organic materials (Frenkel) and inorganic materials (Wannier-Mott) produce polaritons with different interparticle interaction strength. A hybrid polariton state with distinct excitons provides a potential technological route towards in-situ control of nonlinear behaviour. Here we demonstrate a device in which hybrid polaritons are displayed at ambient temperatures, the excitonic component of which is part Frenkel and part Wannier-Mott, and in which the dominant exciton type can be switched with an applied voltage. The device consists of an open microcavity containing both organic dye and a monolayer of the transition metal dichalcogenide WS$_2$. Our findings offer a perspective for electrically controlled nonlinear polariton devices at room temperature.

cond-mat.mes-hall↗

arXiv2016

Experimental and theoretical analyses of strongly polarized photon emission from non-polar InGaN quantum dots

We present a comprehensive investigation of the polarization properties of non-polar a-plane InGaN quantum dots (QDs) and their origin with statistically significant experimental data and rigorous k.p modelling. The unbiased selection and study of 180 individual QDs allow us to compute an average polarization degree of 0.90, with a standard deviation of only 0.08. When coupled with theoretical insights, we show that a-plane InGaN QDs are highly insensitive to size differences, shape anisotropies, and indium content fluctuations. Furthermore, 91% of the studied QDs exhibit a polarization axis along the crystal [1-100] axis, with the other 9% polarized orthogonal to this direction. When coupled with their ability to emit single-photons, a-plane QDs are good candidates for the generation of linearly polarized single-photons, a feature attractive for quantum cryptography protocols.

cond-mat.mes-hall↗

arXiv2016

Two-dimensional Excitonic Photoluminescence in Graphene on Cu surface

Despite having outstanding electrical properties, graphene is unsuitable for optical devices because of its zero band gap. Here, we report two-dimensional excitonic photoluminescence (PL) from graphene grown on Cu(111) surface, which shows an unexpected remarkably sharp and strong emission near 3.16 eV (full-width at half-maximum $\leq$ 3meV) and multiple emissions around 3.18 eV. As temperature increases, these emissions blue-shift, showing the characteristic negative thermal coefficient of graphene. Observed PLs originate from significantly suppressed dispersion of excited electrons in graphene caused by hybridization of graphene $π$ and Cu d orbitals of the 1st and 2nd Cu layers at a shifted saddle point 0.525(M+K) of Brillouin zone. This finding provides a new pathway to engineering novel optoelectronic graphene devices, whilst maintaining the outstanding electrical properties of graphene.

cond-mat.mes-hall↗

arXiv2016

An ultrafast polarised single photon source at 220 K

A crucial requirement for the realisation of efficient and scalable on-chip quantum communication is an ultrafast polarised single photon source operating beyond the Peltier cooling barrier of 200 K. While a few systems based on different materials and device structures have achieved single photon generation above this threshold, there has been no report of single quantum emitters with deterministic polarisation properties at the same high temperature conditions. Here, we report the first device to simultaneously achieve single photon emission with a g(2)(0) of only 0.21, a high polarisation degree of 0.80, a fixed polarisation axis determined by the underlying crystallography, and a GHz repetition rate with a radiative lifetime of 357 ps at 220 K. The temperature insensitivity of these properties, together with the simple planar growth method, and absence of complex device geometries, makes this system an excellent candidate for on-chip applications in integrated systems.

cond-mat.mes-hall↗

arXiv2016

Ultrafast, polarized, single-photon emission from m-plane InGaN Quantum Dots on GaN nanowires

We demonstrate single photon emission from self-assembled m-plane InGaN quantum dots (QDs) embedded on the side-walls of GaN nanowires. A combination of electron microscopy, cathodoluminescence, time-resolved micro-PL and photon autocorrelation experiments give a thorough evaluation of the QDs structural and optical properties. The QD exhibits anti-bunched emission up to 100 K, with a measured autocorrelation function of g^2(0) = 0.28 (0.03) at 5 K. Studies on a statistically significant number of QDs show that these m-plane QDs exhibit very fast radiative lifetimes (260 +/- 55 ps) suggesting smaller internal fields than any of the previously reported c-plane and a-plane QDs. Moreover, the observed single photons are almost completely linearly polarized aligned perpendicular to the crystallographic c-axis with a degree of linear polarization of 0.84 +/- 0.12. Such InGaN QDs incorporated in a nanowire system meet many of the requirements for implementation into quantum information systems and could potentially open the door to wholly new device concepts.

cond-mat.mes-hall↗

arXiv2016

Room-temperature exciton-polaritons with two-dimensional WS2

Two-dimensional transition metal dichalcogenides exhibit strong optical transitions with significant potential for optoelectronic devices. In particular they are suited for cavity quantum electrodynamics in which strong coupling leads to polariton formation as a root to realisation of inversionless lasing, polariton condensationand superfluidity. Demonstrations of such strongly correlated phenomena to date have often relied on cryogenic temperatures, high excitation densities and were frequently impaired by strong material disorder. At room-temperature, experiments approaching the strong coupling regime with transition metal dichalcogenides have been reported, but well resolved exciton-polaritons have yet to be achieved. Here we report a study of monolayer WS$_2$ coupled to an open Fabry-Perot cavity at room-temperature, in which polariton eigenstates are unambiguously displayed. In-situ tunability of the cavity length results in a maximal Rabi splitting of $\hbar Ω_{\rm{Rabi}} = 70$ meV, exceeding the exciton linewidth. Our data are well described by a transfer matrix model appropriate for the large linewidth regime. This work provides a platform towards observing strongly correlated polariton phenomena in compact photonic devices for ambient temperature applications.

cond-mat.mes-hall↗

arXiv2016

Strong exciton-photon coupling with colloidal nanoplatelets in an open microcavity

Colloidal semiconductor nanoplatelets exhibit quantum size effects due to their thickness of only few monolayers, together with strong optical band-edge transitions facilitated by large lateral extensions. In this article we demonstrate room temperature strong coupling of the light and heavy hole exciton transitions of CdSe nanoplatelets with the photonic modes of an open planar microcavity. Vacuum Rabi splittings of $66 \pm 1$ meV and $58 \pm 1$ meV are observed for the heavy and light hole excitons respectively, together with a polariton-mediated hybridisation of both transitions. By measuring the concentration of platelets in the film we compute the transition dipole moment of a nanoplatelet exciton to be $μ= (575 \pm 110)$ D. The large oscillator strength and fluorescence quantum yield of semiconductor nanoplatelets provide a perspective towards novel photonic devices, combining polaritonic and spinoptronic effects.

cond-mat.mes-hall↗

arXiv2013

Non-polar (11-20) InGaN quantum dots with short exciton lifetimes grown by metal-organic vapor phase epitaxy

We report on the optical characterization of non-polar a-plane InGaN quantum dots (QDs) grown by metal-organic vapor phase epitaxy using a short nitrogen anneal treatment at the growth temperature. Spatial and spectral mapping of sub-surface QDs have been achieved by cathodoluminescence at 8 K. Microphotoluminescence studies of the QDs reveal resolution limited sharp peaks with typical linewidth of 1 meV at 4.2 K. Time-resolved photoluminescence studies suggest the excitons in these QDs have a typical lifetime of 538 ps, much shorter than that of the c-plane QDs, which is strong evidence of the significant suppression of the internal electric fields.

cond-mat.mtrl-sci↗