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1.
Chemphyschem ; 23(4): e202100809, 2022 Feb 16.
Artículo en Inglés | MEDLINE | ID: mdl-34905640

RESUMEN

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.

2.
Phys Rev Lett ; 124(15): 153602, 2020 Apr 17.
Artículo en Inglés | MEDLINE | ID: mdl-32357066

RESUMEN

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.

3.
Opt Express ; 24(5): 5615-5627, 2016 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-29092383

RESUMEN

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.

4.
Nanoscale ; 15(1): 177-184, 2022 Dec 22.
Artículo en Inglés | MEDLINE | ID: mdl-36472171

RESUMEN

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.

5.
Nat Commun ; 12(1): 706, 2021 Jan 29.
Artículo en Inglés | MEDLINE | ID: mdl-33514731

RESUMEN

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.

6.
Rev Sci Instrum ; 86(8): 083106, 2015 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-26329173

RESUMEN

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.

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