Carlo Bradac

Observation and control of blinking nitrogen-vacancy centres in discrete nanodiamonds

Nitrogen-vacancy colour centres in diamond can undergo strong, spin-sensitive optical transitions under ambient conditions, which makes them attractive for applications in quantum optics, nanoscale magnetometry and biolabelling. Although nitrogen-vacancy centres have been observed in aggregated detonation nanodiamonds and milled nanodiamonds, they have not been observed in very small isolated nanodiamonds. Here, we report the first direct observation of nitrogen-vacancy centres in discrete 5-nm nanodiamonds at room temperature, including evidence for intermittency in the luminescence (blinking) from the nanodiamonds. We also show that it is possible to control this blinking by modifying the surface of the nanodiamonds.

Prediction and Measurement of the Size-Dependent Stability of Fluorescence in Diamond over the Entire Nanoscale

Fluorescent defects in noncytotoxic diamond nanoparticles are candidates for qubits in quantum computing, optical labels in biomedical imaging, and sensors in magnetometry. For each application these defects need to be optically and thermodynamically stable and included in individual particles at suitable concentrations (singly or in large numbers). In this Letter, we combine simulations, theory, and experiment to provide the first comprehensive and generic prediction of the size, temperature, and nitrogen-concentration-dependent stability of optically active N-V defects in nanodiamonds.

Emission and nonradiative decay of nanodiamond NV centers in a low refractive index environment

The nitrogen vacancy (NV) center is the most widely studied single optical defect in diamond with great potential for applications in quantum technologies. Development of practical single-photon devices requires an understanding of the emission under a range of conditions and environments. In this work, we study the properties of a single NV center in nanodiamonds embedded in an air-like silica aerogel environment which provides a new domain for probing the emission behavior of NV centers in nanoscale environments. In this arrangement, the emission rate is governed primarily by the diamond crystal lattice with negligible contribution from the surrounding environment. This is in contrast to the conventional approach of studying nanodiamonds on a glass coverslip. We observe an increase in the mean lifetime due to the absence of a dielectric interface near the emitting dipoles and a distribution arising from the irregularities in the nanodiamond geometry. Our approach results in the estimation of the mean quantum efficiency (~0.7) of the nanodiamond NV emitters.

Modification of spontaneous emission from nanodiamond colour centres on a structured surface

Colour centres in diamond are promising candidates as a platform for quantum technologies and biomedical imaging based on spins and/or photons. Controlling the emission properties of colour centres in diamond is a key requirement for the development of efficient single-photon sources having high collection efficiency. A number of groups have achieved an enhancement in the emission rate over narrow wavelength ranges by coupling single emitters in nanodiamond crystals to resonant electromagnetic structures. In this paper, we characterize in detail the spontaneous emission rates of nitrogen-vacancy centres at various locations on a structured substrate. We found a factor of 1.5 average enhancement of the total emission rate when nanodiamonds are on an opal photonic crystal surface, and observed changes in the lifetime distribution. We present a model for explaining these observations and associate the lifetime properties with dipole orientation and polarization effects.Colour centres in diamond are promising candidates as a platform for quantum technologies and biomedical imaging based on spins and/or photons. Controlling the emission properties of colour centres in diamond is a key requirement for developing efficient single photon sources with high collection efficiency. A number of groups have produced enhancement in the emission rate over narrow wavelength ranges by coupling single emitters in nanodiamond crystals to resonant electromagnetic structures. Here we characterise in detail the spontaneous emission rates of nitrogen-vacancy centres positioned in various locations on a structured substrate. We show an average factor of 1.5 enhancement of the total emission rate when nanodiamonds are on an opal photonic crystal surface, and observe changes in the lifetime distribution. We present a model to explain these observations and associate the lifetime properties with dipole orientation and polarization effects.

Cooperatively enhanced dipole forces from artificial atoms in trapped nanodiamonds

Since the early work by Ashkin in 1970, optical trapping has become one of the most powerful tools for manipulating small particles, such as micron sized beads or single atoms. The optical trapping mechanism is based on the interaction energy of a dipole and the electric field of the laser light. In atom trapping, the dominant contribution typically comes from the allowed optical transition closest to the laser wavelength, whereas for mesoscopic particles it is given by the bulk polarizability of the material. These two different regimes of optical trapping have coexisted for decades without any direct link, resulting in two very different contexts of applications: one being the trapping of small objects mainly in biological settings, the other one being dipole traps for individual neutral atoms in the field of quantum optics. Here we show that for nanoscale diamond crystals containing artificial atoms, so-called nitrogen vacancy (NV) color centers, both regimes of optical trapping can be observed at the same time even in a noisy liquid environment. For wavelengths in the vicinity of the zero-phonon line transition of the color centers, we observe a significant modification (

Two-photon polarization-selective etching of emergent nano-structures on diamond surfaces

10\%

Processing 15-nm Nanodiamonds Containing Nitrogen-vacancy Centres for Single-molecule FRET

) of the overall trapping strength. Most remarkably, our experimental findings suggest that owing to the large number of artificial atoms, collective effects greatly contribute to the observed trapping strength modification. Our approach adds the powerful atomic-physics toolbox to the field of nano-manipulation.

Nano-assembly of nanodiamonds by conjugation to actin filaments.

Optical techniques have advanced considerably in recent years to enable processing of surfaces with a resolution less than the wavelength of light. Despite the highly selective nature of light-matter interactions, however, efforts to increase resolution to the scale of single atoms are hampered by rapid and efficient dissipation of the absorbed energy to the surrounding matrix. Here we show that two-photon surface excitation using ultraviolet light provides a method for selectively removing carbon from diamond surfaces. Polished surfaces etched by this method develop ultra-deep subwavelength structures with morphologies dependent on the polarization of the incident laser with respect to the crystal axes. As well as revealing a practical and versatile method for nano-patterning of diamond surfaces, we show that the results comprise mesoscopic evidence for bond scission via a highly localized optical interaction that may lead to the development of new optical approaches for ultra-nanoscale (<10 nm) surface structuring.

Wide-field time-gated photoluminescence microscopy for fast ultrahigh-sensitivity imaging of photoluminescent probes.

Colour centres in nanodiamonds have many properties such as chemical and physical stability, biocompatibility, straightforward surface functionalisation as well as bright and stable photoluminescence, which make them attractive for biological applications. Here we examine the use of fluorescent nanodiamonds containing a single nitrogen-vacancy (NV) centre, as an alternative nano-label over conventional fluorophores. We describe a series of chemical treatments and air oxidation to reliably produce small (~15 nm) oxidised nanodiamonds suitable for applications in bioscience. We use Forster resonance energy transfer to measure the coupling efficiency from a single NV centre in a selected nanodiamond to an IRDye 800CW dye molecule absorbed onto the surface. Our single-molecule Forster resonance energy transfer analysis, based on fluorescence lifetime measurements, locates the position of the photostable NV centre deep within the core of the nanodiamond.

Room-temperature spontaneous superradiance from single diamond nanocrystals.

Fluorescent nanodiamonds (NDs) are remarkable objects. They possess unique mechanical and optical properties combined with high surface areas and controllable surface reactivity. They are non-toxic and hence suited for use in biological environments. NDs are also readily available and commercially inexpensive. Here, the exceptional capability of controlling and tailoring their surface chemistry is demonstrated. Small, bright diamond nanocrystals (size ˜30 nm) are conjugated to protein filaments of actin (length ˜3-7 µm). The conjugation to actin filaments is extremely selective and highly target-specific. These unique features, together with the relative simplicity of the conjugation-targeting method, make functionalised nanodiamonds a powerful and versatile platform in biomedicine and quantum nanotechnologies. Applications ranging from using NDs as superior biological markers to, potentially, developing novel bottom-up approaches for the fabrication of hybrid quantum devices that would bridge across the bio/solid-state interface are presented and discussed.