Magnetic measurements on micrometer-sized samples under high pressure using designed NV centers.

Pressure can be used to tune the interplay among structural, electronic, and magnetic interactions in materials. High pressures are usually applied in the diamond anvil cell, making it difficult to study the magnetic properties of a micrometer-sized sample. We report a method for spatially resolved optical magnetometry based on imaging a layer of nitrogen-vacancy (NV) centers created at the surface of a diamond anvil. We illustrate the method using two sets of measurements realized at room temperature and low temperature, respectively: the pressure evolution of the magnetization of an iron bead up to 30 gigapascals showing the iron ferromagnetic collapse and the detection of the superconducting transition of magnesium dibromide at 7 gigapascals.

Infrared laser threshold magnetometry with a NV doped diamond intracavity etalon.

We propose a hybrid laser system consisting of a semiconductor external cavity laser associated to an intra-cavity diamond etalon doped with nitrogen-vacancy color centers. We consider laser emission tuned to the infrared absorption line that is enhanced under the magnetic field dependent nitrogen-vacancy electron spin resonance and show that this architecture leads to a compact solid-state magnetometer that can be operated at room-temperature. The sensitivity to the magnetic field limited by the photonshot-noise of the output laser beam is estimated to be less than 1 pT/Hz. Unlike usual NV center infrared magnetometry, this method would not require an external frequency stabilized laser. Since the proposed system relies on the competition between the laser threshold and an intracavity absorption, such laser-based optical sensor could be easily adapted to a broad variety of sensing applications based on absorption spectroscopy.

Optical Magnetometry of Single Biocompatible Micromagnets for Quantitative Magnetogenetic and Magnetomechanical Assays.

The mechanical manipulation of magnetic nanoparticles is a powerful approach to probing and actuating biological processes in living systems. Implementing this technique in high-throughput assays can be achieved using biocompatible micromagnet arrays. However, the magnetic properties of these arrays are usually indirectly inferred from simulations or Stokes drag measurements, leaving unresolved questions about the actual profile of the magnetic fields at the micrometer scale and the exact magnetic forces that are applied. Here, we exploit the magnetic field sensitivity of nitrogen-vacancy color centers in diamond to map the 3D stray magnetic field produced by a single soft ferromagnetic microstructure. By combining this wide-field optical magnetometry technique with magneto-optic Kerr effect microscopy, we fully analyze the properties of the micromagnets, including their magnetization saturation and their size-dependent magnetic susceptibility. We further show that the high magnetic field gradients produced by the micromagnets, greater than 104 T·m-1 under an applied magnetic field of about 100 mT, enables the manipulation of magnetic nanoparticles smaller than 10 nm inside living cells. This work paves the way for quantitative and parallelized experiments in magnetogenetics and magnetomechanics in cell biology.

Stimulated emission depletion microscopy resolves individual nitrogen vacancy centers in diamond nanocrystals.

Nitrogen-vacancy (NV) color centers in nanodiamonds are highly promising for bioimaging and sensing. However, resolving individual NV centers within nanodiamond particles and the controlled addressing and readout of their spin state has remained a major challenge. Spatially stochastic super-resolution techniques cannot provide this capability in principle, whereas coordinate-controlled super-resolution imaging methods, like stimulated emission depletion (STED) microscopy, have been predicted to fail in nanodiamonds. Here we show that, contrary to these predictions, STED can resolve single NV centers in 40-250 nm sized nanodiamonds with a resolution of ≈10 nm. Even multiple adjacent NVs located in single nanodiamonds can be imaged individually down to relative distances of ≈15 nm. Far-field optical super-resolution of NVs inside nanodiamonds is highly relevant for bioimaging applications of these fluorescent nanolabels. The targeted addressing and readout of individual NV(-) spins inside nanodiamonds by STED should also be of high significance for quantum sensing and information applications.

Single KTP nanocrystals as second-harmonic generation biolabels in cortical neurons.

We report an efficient colloidal synthesis of KTiOPO4 (KTP) nanocrystals with excellent crystallinity and the direct observation of optical second-harmonic generation (SHG) from discrete KTP nanocrystals in neurons cultured from mammalian brain cortex. Direct internalization and monitoring of these nanoparticles was successfully achieved without limitations from cytotoxicity, bleaching and blinking emission.

Near-field optical microscopy with a nanodiamond-based single-photon tip.

We introduce a point-like scanning single-photon source that operates at room temperature and offers an exceptional photostability (no blinking, no bleaching). This is obtained by grafting in a controlled way a diamond nanocrystal (size around 20 nm) with single nitrogen-vacancy color-center occupancy at the apex of an optical probe. As an application, we image metallic nanostructures in the near-field, thereby achieving a near-field scanning single-photon microscopy working at room temperature on the long term. Our work may be of importance to various emerging fields of nanoscience where an accurate positioning of a quantum emitter is required such as for example quantum plasmonics.

Coherent nonlinear emission from a single KTP nanoparticle with broadband femtosecond pulses.

We demonstrate that the intensity of the second harmonic (SH) generated in KTiOPO(4) nanoparticles excited with femtosecond laser pulses increases with decreasing duration of the infrared pump pulses. The SH intensity scales, approximately, as the inverse of the laser pulse duration ranging between 13 fs and 200 fs. The SH intensity enhancement requires careful compensation of the high-order spectral phase, being achieved with a genetic algorithm. Using ultrashort laser pulses improves the signal-to-noise ratio and will allow the detection of 10-nm size particles. Finally, we demonstrate that the spectrum of broadband (100 nm) pulses can be shaped to generate non-degenerate sum-frequency mixing. This opens up access to the polarization degrees of freedom of this second-order nonlinear process at the nanoscale.

Delayed-choice test of quantum complementarity with interfering single photons.

We report an experimental test of quantum complementarity with single-photon pulses sent into a Mach-Zehnder interferometer with an output beam splitter of adjustable reflection coefficient R. In addition, the experiment is realized in Wheeler's delayed-choice regime. Each randomly set value of R allows us to observe interference with visibility V and to obtain incomplete which-path information characterized by the distinguishability parameter D. Measured values of V and D are found to fulfill the complementarity relation V2+D2 < or =1.

Diamond nanocrystals hosting single nitrogen-vacancy color centers sorted by photon-correlation near-field microscopy.

Diamond nanocrystals containing highly photoluminescent color centers are attractive, nonclassical, and near-field light sources. For near-field applications, the size of the nanocrystal is crucial, since it defines the optical resolution. Nitrogen-vacancy (NV) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamonds with sizes down to 25 nm can hold a single NV color center with bright and stable photoluminescence.

Experimental realization of Wheeler's delayed-choice gedanken experiment.

Wave-particle duality is strikingly illustrated by Wheeler's delayed-choice gedanken experiment, where the configuration of a two-path interferometer is chosen after a single-photon pulse has entered it: Either the interferometer is closed (that is, the two paths are recombined) and the interference is observed, or the interferometer remains open and the path followed by the photon is measured. We report an almost ideal realization of that gedanken experiment with single photons allowing unambiguous which-way measurements. The choice between open and closed configurations, made by a quantum random number generator, is relativistically separated from the entry of the photon into the interferometer.

Narrow-band single-photon emission in the near infrared for quantum key distribution.

We present a detailed study of photophysical properties of single color centers in natural diamond samples emitting in the near infrared under optical excitation. Photoluminescence of these single emitters has several striking features, including narrow-band (FWHM 2 nm) fully polarized emission around 780 nm, a short excited-state lifetime of about 2 ns, and perfect photostability at room temperature under our excitation conditions. Development of a triggered single-photon source relying on this single color center is discussed for application to quantum key distribution.

Simple interferometric technique for generation of a radially polarized light beam.

We present a theoretical and experimental investigation of an interferometric technique for converting a linearly polarized Gaussian beam into a radially polarized doughnut beam. The experimental setup accomplishes the coherent summation of two orthogonally polarized TEM01 and TEM10 beams that are obtained from the transformation of a TEM00 beam by use of a simple binary diffractive optical element. We have shown that the degree of radial polarization is maximum at a given distance from the interferometer output port that depends on the diameter of the incident beam at the interferometer input port.

In situ diagnostics of the crystalline nature of single organic nanocrystals by nonlinear microscopy.

We elucidate the crystalline nature and the three-dimensional orientation of isolated organic nanocrystals embedded in a sol-gel matrix, using a polarized nonlinear microscopy technique that combines two-photon fluorescence and second harmonic generation. This technique allows the distinction between monocrystalline structures and nanoscale polycrystalline aggregates responsible for incoherent second harmonic signals.