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

Quantum plasmonics: second-order coherence of surface plasmons launched by quantum emitters into a metallic film

We address the issue of the second-order coherence of single surface plasmons launched by a quantum source of light into extended gold films. The quantum source of light is made of a scanning fluorescent nanodiamond hosting five nitrogen-vacancy (NV) color centers. By using a specially designed microscopy that combines near-field optics with far-field leakage-radiation microscopy in the Fourier space and adapted spatial filtering, we find that the quantum statistics of the initial source of light is preserved after conversion to surface plasmons and propagation along the polycrystalline gold film.Comment: Second version with minor changes made to comply with Referees' comments. Editorially approved for publication in Phys. Rev. B on 22 June 201

Switchable ErSc2N rotor within a C80 fullerene cage: An EPR and photoluminescence excitation study

Systems exhibiting both spin and orbital degrees of freedom, of which Er3+ is one, can offer mechanisms for manipulating and measuring spin states via optical excitations. Motivated by the possibility of observing photoluminescence and electron paramagnetic resonance from the same species located within a fullerene molecule, we initiated an EPR study of Er3+ in ErSc2N@C80. Two orientations of the ErSc2N rotor within the C80 fullerene are observed in EPR, consistent with earlier studies using photoluminescence excitation (PLE) spectroscopy. For some crystal field orientations, electron spin relaxation is driven by an Orbach process via the first excited electronic state of the 4I_15/2 multiplet. We observe a change in the relative populations of the two ErSc2N configurations upon the application of 532 nm illuminations, and are thus able to switch the majority cage symmetry. This photoisomerisation, observable by both EPR and PLE, is metastable, lasting many hours at 20 K.Comment: 4 pages, 4 figure

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

Wave-mixing origin and optimization in single and compact aluminum nanoantennas

The outstanding optical properties for plasmon resonances in noble metal nanoparticles enable the observation of non-linear optical processes such as second-harmonic generation (SHG) at the nanoscale. Here, we investigate the SHG process in single rectangular aluminum nanoantennas and demonstrate that i) a doubly resonant regime can be achieved in very compact nanostructures, yielding a 7.5 enhancement compared to singly resonant structures and ii) the $\chi_{\perp\perp\perp}$ local surface and $\gamma_{bulk}$ nonlocal bulk contributions can be separated while imaging resonant nanostructures excited by a tightly focused beam, provided the $\chi_{\perp\parallel\parallel}$ local surface is assumed to be zero, as it is the case in all existing models for metals. Thanks to the quantitative agreement between experimental and simulated far-field SHG maps, taking into account the real experimental configuration (focusing and substrate), we identify the physical origin of the SHG in aluminum nanoantennas as arising mainly from $\chi_{\perp\perp\perp}$ local surface sources

Nanoscale magnetic field mapping with a single spin scanning probe magnetometer

We demonstrate quantitative magnetic field mapping with nanoscale resolution, by applying a lock-in technique on the electron spin resonance frequency of a single nitrogen-vacancy defect placed at the apex of an atomic force microscope tip. In addition, we report an all-optical magnetic imaging technique which is sensitive to large off-axis magnetic fields, thus extending the operation range of diamond-based magnetometry. Both techniques are illustrated by using a magnetic hard disk as a test sample. Owing to the non-perturbing and quantitative nature of the magnetic probe, this work should open up numerous perspectives in nanomagnetism and spintronics

Sublimation of the Endohedral Fullerene Er3N@C80

The heat of sublimation of the endohedral metallofullerene Er3N@C80 was measured via Knudsen effusion mass spectrometry. The large molecule consists of a C80 fullerene cage which is stabilized by comprising a complex of three erbium atoms bounded to a nitrogen atom and has a mass of 1475 amu. The mass spectrum at a temperature of 1045 K and the relative intensities of the thermal fractions of Er3N@C80 are provided. We also discuss possible thermal decomposition processes for these particles. By measuring the quantity of evaporated molecules in thermal equilibrium through a quadrupole mass spectrometer in a temperature range between 782 K and 1128 K, a value for the sublimation enthalpy of Hsub = 237 +-7 kJ/mol is obtained from the second law method.Comment: Phys. Chem. Chem. Phys., 2010, Advance Articl

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