arXiv subjects

Alex S. Clark

Publications and source records attributed to Alex S. Clark.

35 records · Page 2Linked to original sources

arXiv2020

Coherent characterisation of a single molecule in a photonic black box

Extinction spectroscopy is a powerful tool for demonstrating the coupling of a single quantum emitter to a photonic structure. However, it can be challenging in all but the simplest of geometries to deduce an accurate value of the coupling efficiency from the measured spectrum. Here we develop a theoretical framework to deduce the coupling efficiency from the measured transmission and reflection spectra without precise knowledge of the photonic environment. We then consider the case of a waveguide interrupted by a transverse cut in which an emitter is placed. We apply that theory to a silicon nitride waveguide interrupted by a gap filled with anthracene that is doped with dibenzoterrylene molecules. We describe the fabrication of these devices, and experimentally characterise the waveguide coupling of a single molecule in the gap.

quant-ph↗

arXiv2020

Single-photon-level sub-Doppler pump-probe spectroscopy of rubidium

We propose and demonstrate pump-probe spectroscopy of rubidium absorption which reveals the sub-Doppler hyperfine structure of the $^{5}$S$_{1/2} \leftrightarrow$ $^{5}$P$_{3/2}$ (D2) transitions. The counter propagating pump and probe lasers are independently tunable in frequency, with the probe operating at the single-photon-level. The two-dimensional spectrum measured as the laser frequencies are scanned shows fluorescence, Doppler-broadened absorption dips and sub-Doppler features. The detuning between the pump and probe lasers allows compensation of the Doppler shift for all atomic velocities in the room temperature vapor, meaning we observe sub-Doppler features for all atoms in the beam. We detail a theoretical model of the system which incorporates fluorescence, saturation effects and optical pumping and compare this with the measured spectrum, finding a mean absolute percentage error of 4.17\%. In the future this technique could assist in frequency stabilization of lasers, and the single-photon-level probe could be replaced by a single photon source.

physics.atom-ph↗

arXiv2020

Polymer-encapsulated organic nanocrystals for single photon emission

We demonstrate an emulsion-polymerisation technique to embed dibenzoterrylene-doped anthracene nanocrystals in polymethyl methacrylate (PMMA) nanocapsules. The nanocapsules require no further protection after fabrication and are resistant to sublimation compared to unprotected anthracene. The room temperature emission from single dibenzoterrylene molecules is stable and when cooled to cryogenic temperatures we see no change in their excellent optical properties compared to existing growth methods. These now robust nanocapsules have potential for surface functionalisation and integration into nanophotonic devices, where the materials used are compatible with incorporation in polymer-based designs.

physics.optics↗

arXiv2020

Phonon-induced optical dephasing in single organic molecules

Organic molecules have recently gained attention as novel sources of single photons. We present a joint experiment--theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single molecule. We observe spectra with a zero-phonon-line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localised vibrational modes of the molecule and a thermal phonon bath, which we include non-perturbatively, and is able capture all observed features. For resonant driving we measure Rabi oscillations that become increasingly damped with temperature, which our model naturally reproduces. Our results constitute an essential characterisation of the photon coherence of these promising molecules, paving the way towards their use in future quantum information applications.

quant-ph↗

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

Efficient excitation of dye molecules for single photon generation

A reliable photon source is required for many aspects of quantum technology. Organic molecules are attractive for this application because they can have high quantum yield and can be photostable, even at room temperature. To generate a photon with high probability, a laser must excite the molecule efficiently. We develop a simple model for that efficiency and discuss how to optimise it. We demonstrate the validity of our model through experiments on a single dibenzoterrylene (DBT) molecule in an anthracene crystal. We show that the excitation probability cannot exceed 75\% at room temperature, but can increase to over 99\% if the sample is cooled to liquid nitrogen temperature. The possibility of high photon generation efficiency with only modest cooling is a significant step towards a reliable photon source that is simple and practical.

quant-ph↗

arXiv2016

Quantum dynamics of a driven two-level molecule with variable dephasing

The longitudinal ($Γ_1$) and transverse ($Γ_2$) decay rates of a two-level quantum system have profound influence on its evolution. Atomic systems with $Γ_2=\tfrac{1}{2}Γ_1$ have been studied extensively, but with the rise of solid-state quantum devices it is also important to consider the effect of stronger transverse relaxation due to interactions with the solid environment. Here we study the quantum dynamics of a single organic dye molecule driven by a laser. We measure the variation of $Γ_2$ with temperature and determine the activation energy for thermal dephasing of the optical dipole. Then we measure the second-order correlation function $g^{(2)}(τ)$ of the light emitted by the molecule for various ratios $Γ_2/Γ_1$ and saturation parameters $S$. We show that the general solution to the optical Bloch equations accurately describes the observed quantum dynamics over a wide range of these parameters, and we discuss the limitations of the various approximate expressions for $g^{(2)}(τ)$ that appear in the literature.

quant-ph↗

arXiv2016

A stable, single-photon emitter in a thin organic crystal for application to quantum-photonic devices

Single organic molecules offer great promise as bright, reliable sources of identical single photons on demand, capable of integration into solid-state devices. It has been proposed that such molecules in a crystalline organic matrix might be placed close to an optical waveguide for this purpose, but so far there have been no demonstrations of sufficiently thin crystals, with a controlled concentration of suitable dopant molecules. Here we present a method for growing very thin anthracene crystals from super-saturated vapour, which produces crystals of extreme flatness and controlled thickness. We show how this crystal can be doped with a widely adjustable concentration of dibenzoterrylene (DBT) molecules and we examine the optical properties of these molecules to demonstrate their suitability as quantum emitters in nanophotonic devices. Our measurements show that the molecules are available in the crystal as single quantum emitters, with a well-defined polarisation relative to the crystal axes, making them amenable to alignment with optical nanostructures. We find that the radiative lifetime and saturation intensity vary little within the crystal and are not in any way compromised by the unusual matrix environment. We show that a large fraction of these emitters are able to deliver more than $10^{12}$ photons without photo-bleaching, making them suitable for real applications.

quant-ph↗

arXiv2014

Optimizing optical Bragg scattering for single-photon frequency conversion

We develop a systematic theory for optimising single-photon frequency conversion using optical Bragg scattering. The efficiency and phase-matching conditions for the desired Bragg scattering conversion as well as spurious scattering and modulation instability are identified. We find that third-order dispersion can suppress unwanted processes, while dispersion above the fourth order limits the maximum conversion efficiency. We apply the optimisation conditions to frequency conversion in highly nonlinear fiber, silicon nitride waveguides and silicon nanowires. Efficient conversion is confirmed using full numerical simulations. These design rules will assist the development of efficient quantum frequency conversion between multicolour single photon sources for integration in complex quantum networks.

physics.optics↗

arXiv2014

Bi-photon spectral correlation measurements from a silicon nanowire in the quantum and classical regimes

The growing requirement for photon pairs with specific spectral correlations in quantum optics experiments has created a demand for fast, high resolution and accurate source characterization. A promising tool for such characterization uses the classical stimulated process, in which an additional seed laser stimulates photon generation yielding much higher count rates, as recently demonstrated for a $χ^{(2)}$ integrated source in A.~Eckstein \emph{et al.}, Laser Photon. Rev. \textbf{8}, L76 (2014). In this work we extend these results to $χ^{(3)}$ sources, demonstrating spectral correlation measurements via stimulated four-wave mixing for the first time in a integrated optical waveguide, namely a silicon nanowire. We directly confirm the speed-up due to higher count rates and demonstrate that additional resolution can be gained when compared to traditional coincidence measurements. As pump pulse duration can influence the degree of spectral entanglement, all of our measurements are taken for two different pump pulse widths. This allows us to confirm that the classical stimulated process correctly captures the degree of spectral entanglement regardless of pump pulse duration, and cements its place as an essential characterization method for the development of future quantum integrated devices.

physics.optics↗

arXiv2014

Hybrid photonic circuit for multiplexed heralded single photons

A key resource for quantum optics experiments is an on-demand source of single and multiple photon states at telecommunication wavelengths. This letter presents a heralded single photon source based on a hybrid technology approach, combining high efficiency periodically poled lithium niobate waveguides, low-loss laser inscribed circuits, and fast (>1 MHz) fibre coupled electro-optic switches. Hybrid interfacing different platforms is a promising route to exploiting the advantages of existing technology and has permitted the demonstration of the multiplexing of four identical sources of single photons to one output. Since this is an integrated technology, it provides scalability and can immediately leverage any improvements in transmission, detection and photon production efficiencies.

quant-ph↗

arXiv2013

Multi-Colour Quantum Metrology with Entangled Photons

Entangled photons can be used to make measurements with an accuracy beyond that possible with classical light. While most implementations of quantum metrology have used states made up of a single colour of photons, we show that entangled states of two colours can show supersensitivity to optical phase and path-length by using a photonic crystal fibre source of photon pairs inside an interferometer. This setup is relatively simple and robust to experimental imperfections. We demonstrate sensitivity beyond the standard quantum limit and show super-resolved interference fringes using entangled states of two, four, and six photons.

quant-ph↗

arXiv2013

Multi-photon absorption limits to heralded single photon sources

Single photons are of paramount importance to future quantum technologies, including quantum communication and computation. Nonlinear photonic devices using parametric processes offer a straightforward route to generating photons, however additional nonlinear processes may come into play and interfere with these sources. Here we analyse these sources in the presence of multi-photon processes for the first time. We conduct experiments in silicon and gallium indium phosphide photonic crystal waveguides which display inherently different nonlinear absorption processes, namely two-photon (TPA) and three-photon absorption (ThPA), respectively. We develop a novel model capturing these diverse effects which is in excellent quantitative agreement with measurements of brightness, coincidence-to-accidental ratio (CAR) and second-order correlation function g(2)(0), showing that TPA imposes an intrinsic limit on heralded single photon sources. We devise a new figure of merit, the quantum utility (QMU), enabling direct comparison and optimisation of single photon sources.

physics.optics↗

arXiv2013

Integrated spatial multiplexing of heralded single photon sources

The non-deterministic nature of photon sources is a key limitation for single photon quantum processors. Spatial multiplexing overcomes this by enhancing the heralded single photon yield without enhancing the output noise. Here the intrinsic statistical limit of an individual source is surpassed by spatially multiplexing two monolithic silicon correlated photon pair sources, demonstrating a 62.4% increase in the heralded single photon output without an increase in unwanted multi-pair generation. We further demonstrate the scalability of this scheme by multiplexing photons generated in two waveguides pumped via an integrated coupler with a 63.1% increase in the heralded photon rate. This demonstration paves the way for a scalable architecture for multiplexing many photon sources in a compact integrated platform and achieving efficient two photon interference, required at the core of optical quantum computing and quantum communication protocols.

quant-ph↗

arXiv2011

Characteristics of Correlated Photon Pairs Generated in Ultra-compact Silicon Slow-light Photonic Crystal Waveguides

We report the characterization of correlated photon pairs generated in dispersion-engineered silicon slow-light photonic crystal waveguides pumped by picosecond pulses. We found that taking advantage of the 15 nm flat-band slow-light window (vg ~ c/30) the bandwidth for correlated photon-pair generation in 96 and 196 \mum long waveguides was at least 11.2 nm; while a 396 \mum long waveguide reduced the bandwidth to 8 nm (only half of the slow-light bandwidth due to the increased impact of phase matching in a longer waveguide). The key metrics for a photon-pair source: coincidence to accidental ratio (CAR) and pair brightness were measured to be a maximum 33 at a pair generation rate of 0.004 pair per pulse in a 196 \mum long waveguide. Within the measurement errors the maximum CAR achieved in 96, 196 and 396 \mum long waveguides is constant. The noise analysis shows that detector dark counts, leaked pump light, linear and nonlinear losses, multiple pair generation and detector jitter are the limiting factors to the CAR performance of the sources.

quant-ph↗

arXiv2011

Slow-light Enhanced Correlated Photon-Pair Generation in Silicon

We report the generation of correlated photon pairs in the telecom C-band, at room temperature, from a dispersion-engineered silicon photonic crystal waveguide. The spontaneous four-wave mixing process producing the photon pairs is enhanced by slow-light propagation enabling an active device length of less than 100 μm. With a coincidence to accidental ratio of 12.8, at a pair generation rate of 0.006 per pulse, this ultra-compact photon pair source is immediately applicable towards scalable quantum information processing realized on-chip.

quant-ph↗

arXiv2008

An All Optical Fibre Quantum Controlled-NOT Gate

We report the first experimental demonstration of an optical controlled-NOT gate constructed entirely in fibre. We operate the gate using two heralded optical fibre single photon sources and find an average logical fidelity of 90% and an average process fidelity of 0.83<F<0.91. On the basis of a simple model we are able to conclude that imperfections are primarily due to the photon sources, meaning that the gate itself works with very high fidelity.

quant-ph↗