Narrow and Stable Single Photon Emission from Dibenzoterrylene in para-Terphenyl Nanocrystals.

Single organic molecules are promising photon sources for quantum technologies. In this work we show photon emission from dibenzoterrylene, a widely used organic emitter, in a new host matrix, para-terphenyl. We present a reprecipitation growth method that produces para-terphenyl nanocrystals which are ideal for integration into nanophotonic devices due to their small size. We characterise the optical properties of dibenzoterrylene in nanocrystals at room and cryogenic temperatures, showing bright, narrow emission from a single molecule. Spectral data on the vibrational energies is presented and a further 25 additional molecules are characterised. This emitter-host combination has potential for quantum technology purposes with wavelengths suitable for interfacing with quantum memories.

Phonon-Induced Optical Dephasing in Single Organic Molecules.

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 organic 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 localized vibrational modes of the molecule and a thermal phonon bath, which we include nonperturbatively, and is able to 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 characterization of the photon coherence of molecules, paving the way to their use in future quantum information applications.

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

Single dibenzoterrylene (DBT) molecules offer great promise as bright, reliable sources of single photons on demand, capable of integration into solid-state devices. It has been proposed that DBT in anthracene 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 the 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 an 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 can be excited more than 1012 times without photo-bleaching, making them suitable for real applications.

Chalcogenide fiber-based distributed temperature sensor with sub-centimeter spatial resolution and enhanced accuracy.

We demonstrate a sub-centimeter spatial resolution fiber-based distributed temperature sensor with enhanced measurement accuracy and reduced acquisition time. Our approach employs time domain analysis of backscattered Stokes and anti-Stokes photons generated via spontaneous Raman scattering in a chalcogenide (ChG) As2S3 fiber for temperature monitoring. The sensor performance is significantly improved by exploiting the high Raman coefficient and increased refractive index of the ChG fiber. We achieve a temperature uncertainty of ± 0.65 °C for a short measurement time of only 5 seconds; whilst the detection uncertainty is less than ± 0.2 °C for a longer integration time of 2 minutes. We also investigate the optimum Stokes and anti-Stokes bands for optimal sensing performance. Our theoretical analysis shows that a small detuning frequency regime from a pump is more suitable for rapid measurements while a large detuning regime provides higher temperature resolution.

Degenerate photon-pair generation in an ultracompact silicon photonic crystal waveguide.

We demonstrate degenerate, correlated photon-pair generation via slow-light-enhanced spontaneous four-wave mixing in a 96 µm long silicon photonic crystal waveguide. Our device represents a more than 50 times smaller footprint than silicon nanowires. We have achieved a coincidence-to-accidental ratio as high as 47 at a photon generation rate of 0.001 pairs per pulse and 14 at a photon generation rate of 0.023 pairs per pulse, which are both higher than the useful level of 10. This demonstration provides a path to generate indistinguishable photons in an ultracompact platform for future quantum photonic technologies.

Single-frame transmission and phase imaging using off-axis holography with undetected photons.

Imaging with undetected photons relies upon nonlinear interferometry to extract the spatial image from an infrared probe beam and reveal it in the interference pattern of an easier-to-detect visible beam. Typically, the transmission and phase images are extracted using phase-shifting techniques and combining interferograms from multiple frames. Here we show that off-axis digital holography enables reconstruction of both transmission and phase images at the infrared wavelength from a single interferogram, and hence a single frame, recorded in the visible. This eliminates the need for phase stepping and multiple acquisitions, thereby greatly reducing total measurement time for imaging with long acquisition times at low flux or enabling video-rate imaging at higher flux. With this single-frame acquisition technique, we are able to reconstruct transmission images of an object in the infrared beam with a signal-to-noise ratio of 3.680 ± 0.004 at 10 frames per second, and record a dynamic scene in the infrared beam at 33 frames per second.

Mode multiplexed single-photon and classical channels in a few-mode fiber.

We classically measure the entire propagation matrix of a few-mode fiber and use a spatial light modulator to undo modal mixing and recover single-photons launched onto each of the eigenmodes of the fiber at one end, but arriving as mixed modal superpositions at the other. We exploit the orthogonality of these modal channels to improve the isolation between a quantum and classical channel launched onto different spatial and polarization modes at different wavelengths. The spatial diversity of the channels provides an additional 35dB of isolation in addition to that provided by polarization and wavelength.

Photon pair generation in a silicon micro-ring resonator with reverse bias enhancement.

Photon sources are fundamental components for any quantum photonic technology. The ability to generate high count-rate and low-noise correlated photon pairs via spontaneous parametric down-conversion using bulk crystals has been the cornerstone of modern quantum optics. However, future practical quantum technologies will require a scalable integration approach, and waveguide-based photon sources with high-count rate and low-noise characteristics will be an essential part of chip-based quantum technologies. Here, we demonstrate photon pair generation through spontaneous four-wave mixing in a silicon micro-ring resonator, reporting separately a maximum coincidence-to-accidental (CAR) ratio of 602 ± 37 (for a generation rate of 827kHz), and a maximum photon pair generation rate of 123 MHz ± 11 kHz (with a CAR value of 37). To overcome free-carrier related performance degradations we have investigated reverse biased p-i-n structures, demonstrating an improvement in the pair generation rate by a factor of up to 2 with negligible impact on CAR.

High-efficiency frequency conversion in the single-photon regime.

In this Letter we demonstrate frequency conversion in the single-photon regime through Bragg-scattering four-wave mixing with near-unit efficiency in a 750 m long commercially available dispersion-engineered highly nonlinear fiber, where all photons and pump laser frequencies are in the low-loss telecommunications band. We achieve 99.1%±4.9% downconversion and 98.0%±5.0% upconversion of photons by 12 nm using a weak coherent state with an average input of 0.27 photons per detection gate window.

Heralded single-photon source in a III-V photonic crystal.

In this Letter we demonstrate heralded single-photon generation in a III-V semiconductor photonic crystal platform through spontaneous four-wave mixing. We achieve a high brightness of 3.4×10(7) pairs·s(-1) nm(-1) W(-1) facilitated through dispersion engineering and the suppression of two-photon absorption in the gallium indium phosphide material. Photon pairs are generated with a coincidence-to-accidental ratio over 60 and a low g(2) (0) of 0.06 proving nonclassical operation in the single photon regime.

Multicolor 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 color of photons, we show that entangled states of two colors can show supersensitivity to optical phase and path length by using a photonic crystal fiber 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 superresolved interference fringes using entangled states of two, four, and six photons.

Emission enhancement of erbium in a reverse nanofocusing waveguide.

Since Purcell's seminal report 75 years ago, electromagnetic resonators have been used to control light-matter interactions to make brighter radiation sources and unleash unprecedented control over quantum states of light and matter. Indeed, optical resonators such as microcavities and plasmonic antennas offer excellent control but only over a limited spectral range. Strategies to mutually tune and match emission and resonator frequency are often required, which is intricate and precludes the possibility of enhancing multiple transitions simultaneously. In this letter, we report a strong radiative emission rate enhancement of Er3+-ions across the telecommunications C-band in a single plasmonic waveguide based on the Purcell effect. Our gap waveguide uses a reverse nanofocusing approach to efficiently enhance, extract and guide emission from the nanoscale to a photonic waveguide while keeping plasmonic losses at a minimum. Remarkably, the large and broadband Purcell enhancement allows us to resolve Stark-split electric dipole transitions, which are typically only observed under cryogenic conditions. Simultaneous radiative emission enhancement of multiple quantum states is of great interest for photonic quantum networks and on-chip data communications.

Low Raman-noise correlated photon-pair generation in a dispersion-engineered chalcogenide As2S3 planar waveguide.

We demonstrate low Raman-noise correlated photon-pair generation in a dispersion-engineered 10 mm As2S3 chalcogenide waveguide at room temperature. We show a coincidence-to-accidental ratio (CAR) of 16.8, a 250 times increase compared with previously published results in a chalcogenide waveguide, with a corresponding brightness of 3×10(5) pairs·s(-1)·nm(-1) generated at the chip. Dispersion engineering of our waveguide enables photon passbands to be placed in the low spontaneous Raman scattering (SpRS) window at 7.4 THz detuning from the pump. This Letter shows the potential for As2S3 chalcogenide to be used for nonlinear quantum photonic devices.

Uniaxial strain tuning of organic molecule single photon sources.

Organic fluorophores are excellent single photon sources, combining high brightness, lifetime-limited linewidths and useful emission wavelengths. A key factor in their performance as photon emitters is their dynamic frequency tunability, which can be used to render the emission from multiple molecules indistinguishable. In this work we demonstrate dynamic tuning of dibenzoterrylene molecules embedded in anthracene crystals through the application of uniaxial strain fields. By bending a piezoelectric strip in two opposite directions in linear steps, we impose an escalating compressive or tensile strain on the molecular crystals, resulting in two opposite dynamic detunings of the dopant dibenzoterrylene emission wavelength. To validate that the tuning mechanism is strain, we performed a similar measurement using an identical strip that was depolarised by annealing in which the tuning was absent. Finally, we simulated the effect of strain on the dopant dibenzoterrylene emission wavelength by combining molecular dynamics and density functional theory techniques to determine the strain tuning rate which matched well with that found experimentally.

Slow-light enhanced correlated photon pair generation in a silicon photonic crystal waveguide.

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 ultracompact photon pair source paves the way toward scalable quantum information processing realized on-chip.

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.

Growth of optical-quality anthracene crystals doped with dibenzoterrylene for controlled single photon production.

Dibenzoterrylene (DBT) molecules within a crystalline anthracene matrix show promise as quantum emitters for controlled, single photon production. We present the design and construction of a chamber in which we reproducibly grow doped anthracene crystals of optical quality that are several mm across and a few µm thick. We demonstrate control of the DBT concentration over the range 6-300 parts per trillion and show that these DBT molecules are stable single-photon emitters. We interpret our data with a simple model that provides some information on the vapour pressure of DBT.

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 characterisation. A promising tool for such characterisation uses classical stimulated processes, 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 et al. Laser Photon. Rev. 8, L76 (2014). In this work we extend these results to χ(3) integrated sources, directly measuring for the first time the relation between spectral correlation measurements via stimulated and spontaneous four wave mixing in an integrated optical waveguide, a silicon nanowire. We directly confirm the speed-up due to higher count rates and demonstrate that this allows additional resolution to be gained when compared to traditional coincidence measurements without any increase in measurement time. As the pump pulse duration can influence the degree of spectral correlation, 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 correlation regardless of pump pulse duration, and cements its place as an essential characterisation method for the development of future quantum integrated devices.

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 spontaneous four-wave mixing (SFWM) sources in the presence of multi-photon processes. 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 build on these observations to devise a new metric, the quantum utility (QMU), enabling further optimisation of single photon sources.