Single Dibenzoterrylene Molecules Research Articles

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. We also show emission from nanocapsules embedded in a thin layer of titanium dioxide, highlighting their potential for integration into hybrid nanophotonic devices.

Single-Molecule-Doped Crystalline Nanosheets for Delicate Photophysics Studies and Directional Single-Photon-Emitting Devices

Single molecules in solids have been considered as an attractive class of solid-state single quantum systems because they can be chemically synthesized at low cost to have stable narrow transitions at desired wavelengths. Here we report and demonstrate single dibenzoterrylene molecules in crystalline anthracene nanosheets as a robust and versatile solid-state platform for delicate photophysics studies and building blocks of single-photon devices. The high-quality nanosheet sample enables robust studies of delicate single-molecule photophysics at room temperature, including the first real-time observation of single molecule insertion site jump, quantitative measurements of the associated changes of dipole moment orientation and magnitude, unambiguous determination of excitation-power dependent intersystem crossing rate and triplet lifetime. Moreover, we demonstrate the flexible assembly of the nanosheets into a planar antenna device to achieve bright single-molecule emission with a Gaussian emission pattern. The thin thickness, good photostability and mechanical stability make the dibenzoterrylene-in-anthracene nanosheet system an excellent candidate of static quantum nodes in integrated photonic circuit.

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. 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 autocorrelation 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 βWG = 11.6(1.5)%. This type of structure is promising for building new functionality into quantum-photonic circuits, where localized regions of strong emitter-guide coupling can be interconnected by low-loss dielectric guides.

Optimal and robust control of quantum state transfer by shaping the spectral phase of ultrafast laser pulses.

Achieving fast and efficient quantum state transfer is a fundamental task in physics, chemistry and quantum information science. However, the successful implementation of the perfect quantum state transfer also requires robustness under practically inevitable perturbative defects. Here, we demonstrate how an optimal and robust quantum state transfer can be achieved by shaping the spectral phase of an ultrafast laser pulse in the framework of frequency domain quantum optimal control theory. Our numerical simulations of the single dibenzoterrylene molecule as well as in atomic rubidium show that optimal and robust quantum state transfer via spectral phase modulated laser pulses can be achieved by incorporating a filtering function of the frequency into the optimization algorithm, which in turn has potential applications for ultrafast robust control of photochemical reactions.

Spectroscopy of Single Dibenzoterrylene Molecules in para-Dichlorobenzene.

We study single dibenzoterrylene (DBT) molecules embedded in 1,4-dichlorobenzene (para-dichlorobenzene, pDCB) at 1.2 K. Due to the relatively low melting point of pDCB (53 °C), this host-guest system can be easily prepared from the molten phase. Narrow linewidths, stable molecular lines and high saturation count rates of single DBT molecules were observed. For this reason, we consider this host-guest system a promising candidate for the study of interactions of single molecules with other small objects such as waveguides or nanoparticles.

Coupling of single DBT molecules to a graphene monolayer: proof of principle for a graphene nanoruler

ABSTRACTWe report on our recent progress in the study of single Dibenzoterrylene (DBT) molecules as single photon sources and nanoscale probes. We consider DBT molecules embedded in thin anthracene films, a system that allows stable single photon emission both at room and at cryogenic temperatures. We investigate the most important optical properties of the DBT:anthracene system as a whole. We then perform a full statistical study of the coupling between single DBT molecules by measuring the lifetimes of DBT both in the coupled and in the uncoupled case. The experimental results are framed into a simple universal scaling model, where the magnitude of coupling depends solely on universal parameters and on the distance d between the single emitter and the graphene monolayer. We apply this model to infer d and provide a proof of principle for a position ruler at the nanoscale [1].

Single molecule as a local acoustic detector for mechanical oscillators.

A single molecule can serve as a nanometer-sized detector of acoustic strain. Such a nanomicrophone has the great advantage that it can be placed very close to acoustic signal sources and high sensitivities can be achieved. We demonstrate this scheme by monitoring the fluorescence intensity of a single dibenzoterrylene molecule in an anthracene crystal attached to an oscillating tuning fork. The characterization of the vibration amplitude and of the detection sensitivity is a first step towards detection and control of nanomechanical oscillators through optical detection and feedback.

Spectral Diffusion of Single Dibenzoterrylene Molecules in 2,3‐Dimethylanthracene

We study single dibenzoterrylene molecules embedded in the dipolar disordered crystal 2,3-dimethylanthracene at 1.25 K. Broad linewidths (about 1 GHz, ∼30 times broader than in the anthracene crystal), high saturation excitation intensities (∼1000 times larger than in anthracene), as well as strong spectral diffusions are observed. Additionally, spectral jumping is studied by varying the excitation intensity and the temperature. We propose that the spectral diffusion and dynamic disorder in this system arise from the combination of a static disorder with slight reorientations of the methyl groups of the host molecules.

Optical Sensing of Current Dynamics in Organic Light‐Emitting Devices at the Nanometer Scale

Photoluminescence quenching of single dibenzoterrylene (DBT) dye molecules in a polymeric organic light-emitting diode was utilized to analyze the current dynamics at nanometer resolution. The quenching mechanism of single DBT molecules results from an increase in the triplet-state population induced by charge carrier recombination on individual guest molecules. As a consequence of the long triplet-state relaxation time, its population results in a reduced photoluminescence of the dispersed fluorescent dyes. From the decrease in photoluminescence together with photon correlation measurements, we could quantify the local current density and its time-dependent evolution in the vicinity of the single-molecule probe. This optical technique establishes a non-invasive approach to map the time-resolved current density in organic light-emitting diodes on the nanometer scale.

Dye molecules as single-photon sources and large optical nonlinearities on a chip

We point out that individual organic dye molecules, deposited close to optical waveguides on a photonic chip, can act as single-photon sources. A thin silicon nitride strip waveguide is expected to collect 28% of the photons from a single dibenzoterrylene molecule. These molecules can also provide large, localized optical nonlinearities, which are enough to discriminate between one photon or two through a differential phase shift of 2° per photon. This new atom–photon interface may be used as a resource for processing quantum information.

Single dibenzoterrylene molecules in naphthalene and 2,3-dimethylnaphthalene crystals: vibronic spectra

Fluorescence excitation spectra of single dibenzoterrylene (DBT) molecules embedded in naphthalene (N) and 2,3-dimethylnaphthalene (2,3-DMN) crystals were studied at 5 K. The frequencies characterizing the vibronic structure of single DBT molecules in an N crystal agree with the theoretical prediction for the isolated DBT molecule. The 'dipolar' disorder encountered in 2,3-DMN crystals leads to a broad distribution of frequencies of the (0,0) lines of single DBT molecules. Moreover, the observed vibronic frequencies and intensities in the spectrum of DBT in 2,3-DMN crystals are slightly different to those in an N crystal. We conclude that the structure of DBT molecules in a 2,3-DMN crystal is disturbed in comparison with isolated DBT and the main change concerns its central tetracene moiety.

On the photo-stability of single molecules. Dibenzoterrylene in 2,3-dimethylnaphthalene crystals

Fluorescence intensity traces of single dibenzoterrylene molecules in 2,3-dimethylnaphthalene crystals were studied at 270 K. It was found that these molecules are considerably more photo-stable than those of terrylene in the same crystal. Quantum-chemical calculations indicated that the creation of the reactive singlet oxygen state via the triplet state is not probable for dibenzoterrylene, in contrast to terrylene. This reaction provides the first step in typical hydrocarbon oxidation. Therefore, the lack of the triplet channel in the case of dibenzoterrylene, and its domination in the photo-oxidation of terrylene, may explain the different photo-stability of the two compounds.

Single Dibenzoterrylene Molecules in an Anthracene Crystal: Main Insertion Sites

We present a spectroscopic study of the properties of the two principal insertion sites (at 785.1 and 794.3 nm) of single dibenzoterrylene molecules in anthracene single crystals at cryogenic temperatures. We measured the temperature dependence of the line width, the orientation of the transition dipole moments, and the Stark effect. We performed molecular dynamics simulations, which show that one dibenzoterrylene molecule preferably replaces three anthracene molecules. From simulated annealing, we derive the molecular conformations in the most stable insertion sites and the orientations of the transition dipole moments. The good agreement between the spectroscopic results and the simulations allows us to propose unambiguous structures for the two principal spectroscopic sites.

Cover Picture: Single Dibenzoterrylene Molecules in an Anthracene Crystal: Spectroscopy and Photophysics (ChemPhysChem 8/2007)

The cover picture shows a sublimation‐grown anthracene crystal doped with dibenzoterrylene. The deep blue color is the anthracene crystal's intrinsic fluorescence, excited by a mercury line at 365 nm. The red color arises from scattered near‐infrared (785 nm) laser light used to excite dibenzoterrylene. Fluorescence exits the crystal dominantly through the edges, defects and cracks. The bottom of the figure presents a high‐resolution broad‐band fluorescence excitation spectrum of the sample at low temperature around 785 nm. Every sharp line marks the zero‐phonon transition of a single dibenzoterrylene molecule. The group of lines at 12 590 cm−1 is one of the two spectroscopic sites (the “red site”) whose photophysics are studied in the Article by Nicolet et al. on page 1215.

Single Dibenzoterrylene Molecules in an Anthracene Crystal: Spectroscopy and Photophysics

We study single dibenzoterrylene molecules in an anthracene single crystal at 1.4 K in two insertion sites at 785.1 and 794.3 nm. The single-molecule zero-phonon lines are narrow (about 30 MHz), intense (the detected fluorescence rates at saturation reach 100,000 counts s(-1)), and very photostable. The intersystem-crossing yield is extremely low (10(-7) or lower). All of these features are hallmarks of an excellent system for high-resolution spectroscopy and nanoscale probing at cryogenic temperatures.