Photophysics of single nitrogen-vacancy centers in diamond nanocrystals

A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size of 50~nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process

Dependence of the irradiation-induced growth kinetics of satellites on the nanoclusters dimension

A paraître dans NIM B, présenté par G. Rizza (LSI)International audienceIrradiation with MeV gold ions of embedded Au nanoclusters in silica matrix results in the formation of a ring of satellites in its surrounding. We show that changing the initial nanoclusters size modifies both the size and the density of the satellites, and therefore alters their kinetic growth. Finally we discuss the limitation of the ion implantation technique to form a model system to study the satellites kinetic growth and we propose a new approach based on the chemical synthesis of metallic nanoparticles to obtain the proper configuration

Room temperature stable single-photon source

We report on the realization of a stable solid state room temperature source for single photons. It is based on the fluorescence of a single nitrogen-vacancy (NV) color center in a diamond nanocrystal. Antibunching has been observed in the fluorescence light under both continuous and pulsed excitation. Our source delivers 2*10^4 single-photon pulses per second at an excitation repetition rate of 10 MHz. The number of two-photon pulses is reduced by a factor of five compared to strongly attenuated coherent sources.Comment: 7 pages, 10 figures, accepted to the special issue of the European Physical Journal D on "Quantum interference and cryptographic keys: novel physics and advancing technologies", proceedings of the conference QUICK 200

Spin relaxometry of single nitrogen-vacancy defects in diamond nanocrystals for magnetic noise sensing

We report an experimental study of the longitudinal relaxation time ($T_1$) of the electron spin associated with single nitrogen-vacancy (NV) defects hosted in nanodiamonds (ND). We first show that $T_1$ decreases over three orders of magnitude when the ND size is reduced from 100 to 10 nm owing to the interaction of the NV electron spin with a bath of paramagnetic centers lying on the ND surface. We next tune the magnetic environment by decorating the ND surface with Gd$^{3+}$ ions and observe an efficient $T_{1}$-quenching, which demonstrates magnetic noise sensing with a single electron spin. We estimate a sensitivity down to $\approx 14$ electron spins detected within 10 s, using a single NV defect hosted in a 10-nm-size ND. These results pave the way towards $T_1$-based nanoscale imaging of the spin density in biological samples.Comment: Main text with 4 figures together with supplemental informatio

Surface-induced charge state conversion of nitrogen-vacancy defects in nanodiamonds

We present a study of the charge state conversion of single nitrogen-vacancy (NV) defects hosted in nanodiamonds (NDs). We first show that the proportion of negatively-charged NV$^{-}$ defects, with respect to its neutral counterpart NV$^{0}$, decreases with the size of the ND. We then propose a simple model based on a layer of electron traps located at the ND surface which is in good agreement with the recorded statistics. By using thermal oxidation to remove the shell of amorphous carbon around the NDs, we demonstrate a significant increase of the proportion of NV$^{-}$ defects in 10-nm NDs. These results are invaluable for further understanding, control and use of the unique properties of negatively-charged NV defects in diamondComment: 6 pages, 4 figure

Photoluminescence of single colour defects in 50 nm diamond nanocrystals

We used optical confocal microscopy to study optical properties of diamond 50 nm nanocrystals first irradiated with an electron beam, then dispersed as a colloidal solution and finally deposited on a silica slide. At room temperature, under CW laser excitation at a wavelength of 514.5 nm we observed perfectly photostable single Nitrogen-Vacancy (NV) colour defects embedded in the nanocrystals. From the zero-phonon line around 575 nm in the spectrum of emitted light, we infer a neutral NV0 type of defect. Such nanoparticle with intrinsic fluorescence are highly promising for applications in biology where long-term emitting fluorescent bio-compatible nanoprobes are still missing.Comment: proceedings of ICDS 23 conference (23rd International Conference on Defects in Semiconductors, July 24 - July 29, 2005, Awaji Island, Hyogo, Japan); to appear in "Physica B

Positron annihilation in latex templated macroporous silica films: pore size and ortho-positronium escape

International audienceDepth profling of positron annihilation characteristics has been used to investigate the pore size distribution in macroporous PMMA latex templated SiO2 films deposited on glass or Si and prepared with 11-70% porosity. The correlation between the annihilation characteristics shows that o-Ps escape (re-emission) into vacuum occurs in all films with a porosity threshold that is pore size dependent. For 60 ± 2% porosity, the o-Ps reemission yield decreases from ~ 0:25 to ~ 0:11 as the pore size increases from 32 to 75 nm. The o-Ps reemission yield is shown to vary linearly with the specific surface area per mass unit and the slope is independent of pore size, 9:1±0:4 g cm-1. For 32 nm pores, the o-Ps annihilation lifetimes in the films, 17(2)ns and 106(5) ns, show that o-Ps annihilates from micropores with small effective size (1:4 ± 4 nm) and from macropores with large effective size (~ 32 nm). Above the porosity threshold, the o-Ps-escape model predicts the annihilation lifetime in the films to be 19±2 ns. Our results imply that o-Ps effciently detects the microporosity present in the silica walls. At low porosity, its capture into the micropores competes with its capture into the macropores. At higher porosity (when the distance between micropores and macropores become small), this capture into the micropores assists the capture into the macropores

An evolutionary gap in primate default mode network organization

The human default mode network (DMN) is engaged at rest and in cognitive states such as self-directed thoughts. Interconnected homologous cortical areas in primates constitute a network considered as the equivalent. Here, based on a cross-species comparison of the DMN between humans and non-hominoid primates (macaques, marmosets, and mouse lemurs), we report major dissimilarities in connectivity profiles. Most importantly, the medial prefrontal cortex (mPFC) of non-hominoid primates is poorly engaged with the posterior cingulate cortex (PCC), though strong correlated activity between the human PCC and the mPFC is a key feature of the human DMN. Instead, a fronto-temporal resting-state network involving the mPFC was detected consistently across non-hominoid primate species. These common functional features shared between non-hominoid primates but not with humans suggest a substantial gap in the organization of the primate\u27s DMN and its associated cognitive functions

Fast in vivo imaging of SHG nanoprobes with multiphoton light-sheet microscopy

Two-photon light-sheet microscopy (2P-SPIM) provides a unique combination of advantages for fast and deep fluorescence imaging in live tissues. Detecting coherent signals such as second-harmonic generation (SHG) in 2P-SPIM in addition to fluorescence would open further imaging opportunities. However, light-sheet microscopy involves an orthogonal configuration of illumination and detection that questions the ability to detect coherent signals. Indeed, coherent scattering from micron-sized structures occurs predominantly along the illumination beam. By contrast, point-like sources such as SHG nanocrystals can efficiently scatter light in multiple directions and be detected using the orthogonal geometry of a light-sheet microscope. This study investigates the suitability of SHG light-sheet microscopy (SHG-SPIM) for fast imaging of SHG nanoprobes. Parameters that govern the detection efficiency of KTiOPO4 and BaTiO3 nanocrystals using SHG-SPIM are investigated theoretically and experimentally. The effects of incident polarization, detection numerical aperture, nanocrystal rotational motion, and second-order susceptibility tensor symmetries on the detectability of SHG nanoprobes in this specific geometry are clarified. Guidelines for optimizing SHG-SPIM imaging are established, enabling fast in vivo light-sheet imaging combining SHG and two-photon excited fluorescence. Finally, microangiography was achieved in live zebrafish embryos by SHG imaging at up to 180 frames per second and single-particle tracking of SHG nanoprobes in the blood flow