Spin-controlled generation of indistinguishable and distinguishable photons from silicon vacancy centres in silicon carbide.

Quantum systems combining indistinguishable photon generation and spin-based quantum information processing are essential for remote quantum applications and networking. However, identification of suitable systems in scalable platforms remains a challenge. Here, we investigate the silicon vacancy centre in silicon carbide and demonstrate controlled emission of indistinguishable and distinguishable photons via coherent spin manipulation. Using strong off-resonant excitation and collecting zero-phonon line photons, we show a two-photon interference contrast close to 90% in Hong-Ou-Mandel type experiments. Further, we exploit the system's intimate spin-photon relation to spin-control the colour and indistinguishability of consecutively emitted photons. Our results provide a deep insight into the system's spin-phonon-photon physics and underline the potential of the industrially compatible silicon carbide platform for measurement-based entanglement distribution and photonic cluster state generation. Additional coupling to quantum registers based on individual nuclear spins would further allow for high-level network-relevant quantum information processing, such as error correction and entanglement purification.

Sensing Individual Nuclear Spins with a Single Rare-Earth Electron Spin.

Rare-earth related electron spins in crystalline hosts are unique material systems, as they can potentially provide a direct interface between telecom band photons and long-lived spin quantum bits. Specifically, their optically accessible electron spins in solids interacting with nuclear spins in their environment are valuable quantum memory resources. Detection of nearby individual nuclear spins, so far exclusively shown for few dilute nuclear spin bath host systems such as the nitrogen-vacancy center in diamond or the silicon vacancy in silicon carbide, remained an open challenge for rare earths in their host materials, which typically exhibit dense nuclear spin baths. Here, we present the electron spin spectroscopy of single Ce^{3+} ions in a yttrium orthosilicate host, featuring a coherence time of T_{2}=124 µs. This coherent interaction time is sufficiently long to isolate proximal ^{89}Y nuclear spins from the nuclear spin bath of ^{89}Y. Furthermore, it allows for the detection of a single nearby ^{29}Si nuclear spin, native to the host material with ∼5% abundance. This study opens the door to quantum memory applications in rare-earth ion related systems based on coupled environmental nuclear spins, potentially useful for quantum error correction schemes.

Deterministic Single-Ion Implantation of Rare-Earth Ions for Nanometer-Resolution Color-Center Generation.

Single dopant atoms or dopant-related defect centers in a solid state matrix are of particular importance among the physical systems proposed for quantum computing and communication, due to their potential to realize a scalable architecture compatible with electronic and photonic integrated circuits. Here, using a deterministic source of single laser-cooled Pr^{+} ions, we present the fabrication of arrays of praseodymium color centers in yttrium-aluminum-garnet substrates. The beam of single Pr^{+} ions is extracted from a Paul trap and focused down to 30(9) nm. Using a confocal microscope, we determine a conversion yield into active color centers of up to 50% and realize a placement precision of 34 nm.

All-Optical Preparation of Coherent Dark States of a Single Rare Earth Ion Spin in a Crystal.

All-optical addressing and coherent control of single solid-state based quantum bits is a key tool for fast and precise control of ground-state spin qubits. So far, all-optical addressing of qubits was demonstrated only in a very few systems, such as color centers and quantum dots. Here, we perform high-resolution spectroscopic of native and implanted single rare earth ions in solid, namely, a cerium ion in yttrium aluminum garnet (YAG) crystal. We find narrow and spectrally stable optical transitions between the spin sublevels of the ground and excited optical states. Utilizing these transitions we demonstrate the generation of a coherent dark state in electron spin sublevels of a single Ce^{3+} ion in YAG by coherent population trapping.

A compact, diode laser based excitation system for microscopy of NV centers.

We demonstrate that a recently introduced family of direct-emitting green laser diodes is a simple yet efficient light source for excitation of NV centers in diamond. Thanks to their fast (sub-ns) response time, these sources are suitable for a broad variety of measurements, including pulsed optically detected magnetic resonance (ODMR) and fluorescence lifetime imaging. This feature, together with a drastically simplified design, is a significant advantage over the traditional excitation system comprising an Nd: YAG laser switched by an acousto-optic modulator. We introduce a simple design for such a compact laser system and experimentally verify that it enables simultaneous lifetime and ODMR measurements on NV centers. In particular, we find that the NV(-) charge state remains stable in spite of the short excitation wavelength of the new source.

Mapping spin coherence of a single rare-earth ion in a crystal onto a single photon polarization state.

We report on optical detection of a single photostable Ce(3+) ion in an yttrium aluminium garnet (YAG) crystal and on its magneto-optical properties at room temperature. The spin quantum state of the emitting level of a single cerium ion in YAG can be initialized by a circularly polarized laser pulse. Coherent precession of the electron spin is read out by observing temporal behavior of circularly polarized fluorescence of the ion. This implies direct mapping of the spin quantum state of Ce(3+) ion onto the polarization state of the emitted photon and represents the quantum interface between a single spin and a single photon.

Single defect center scanning near-field optical microscopy on graphene.

We present a scanning-probe microscope based on an atomic-size emitter, a single nitrogen-vacancy center in a nanodiamond. We employ this tool to quantitatively map the near-field coupling between the NV center and a flake of graphene in three dimensions with nanoscale resolution. Further we demonstrate universal energy transfer distance scaling between a point-like atomic emitter and a two-dimensional acceptor. Our study paves the way toward a versatile single emitter scanning microscope, which could image and excite molecular-scale light fields in photonic nanostructures or single fluorescent molecules.

Super-resolution fluorescence quenching microscopy of graphene.

Lately, fluorescence quenching microscopy (FQM) has been introduced as a new tool to visualize graphene-based sheets. Even though quenching of the emission from a dye molecule by fluorescence resonance energy transfer (FRET) to graphene happens on the nanometer scale, the resolution of FQM so far is still limited to several hundreds of nanometers due to the Abbe limit restricting the resolution of conventional light microscopy. In this work, we demonstrate an advancement of FQM by using a super-resolution imaging technique for detecting fluorescence of color centers used in FQM. The technique is similar to stimulated emission depletion microscopy (STED). The combined "FRET+STED" technique introduced here for the first time represents a substantial improvement to FQM since it exhibits in principle unlimited resolution while still using light in the visible spectral range. In the present case we demonstrate all-optical imaging of graphene with resolution below 30 nm. The performance of the technique in terms of imaging resolution and contrast is well described by a theoretical model taking into account the general distance dependence of the FRET process and the distance distribution of donor centers with respect to the flake. In addition, the change in lifetime for partially quenched emitters allows extracting the quenching distance from experimental data for the first time.

All-optical high-resolution nanopatterning and 3D suspending of graphene.

We introduce a laser-based technique capable of both imaging and patterning graphene with high spatial resolution. Both tasks are performed in situ using the same confocal microscope. Imaging graphene is based on the recombination of a laser-created electron-hole plasma yielding to a broadband up- and down-converted fluorescence. Patterning is due to burning graphene by local heating causing oxidation and conversion into CO(2). By shaping the laser beam profile using 1D phase-shifting plates and 2D vortex plates we can produce graphene dots below 100 nm in diameter and graphene nanoribbons down to 20 nm in width. Additionally, we demonstrate that this technique can also be applied to freely suspended graphene resulting in freely suspended graphene nanoribbons. We further present a way of freely hanging graphene vertically and imaging it in 3D. Taking advantage of having vertically hanging graphene for the first time, we measure the out-of-plane anisotropy of the upconversion fluorescence.

Ultralong spin coherence time in isotopically engineered diamond.

As quantum mechanics ventures into the world of applications and engineering, materials science faces the necessity to design matter to quantum grade purity. For such materials, quantum effects define their physical behaviour and open completely new (quantum) perspectives for applications. Carbon-based materials are particularly good examples, highlighted by the fascinating quantum properties of, for example, nanotubes or graphene. Here, we demonstrate the synthesis and application of ultrapure isotopically controlled single-crystal chemical vapour deposition (CVD) diamond with a remarkably low concentration of paramagnetic impurities. The content of nuclear spins associated with the (13)C isotope was depleted to 0.3% and the concentration of other paramagnetic defects was measured to be <10(13) cm(-3). Being placed in such a spin-free lattice, single electron spins show the longest room-temperature spin dephasing times ever observed in solid-state systems (T2=1.8 ms). This benchmark will potentially allow observation of coherent coupling between spins separated by a few tens of nanometres, making it a versatile material for room-temperature quantum information processing devices. We also show that single electron spins in the same isotopically engineered CVD diamond can be used to detect external magnetic fields with a sensitivity reaching 4 nT Hz(-1/2) and subnanometre spatial resolution.

Fluorescence and spin properties of defects in single digit nanodiamonds.

This article reports stable photoluminescence and high-contrast optically detected electron spin resonance (ODESR) from single nitrogen-vacancy (NV) defect centers created within ultrasmall, disperse nanodiamonds of radius less than 4 nm. Unexpectedly, the efficiency for the production of NV fluorescent defects by electron irradiation is found to be independent of the size of the nanocrystals. Fluorescence lifetime imaging shows lifetimes with a mean value of around 17 ns, only slightly longer than the bulk value of the defects. After proper surface cleaning, the dephasing times of the electron spin resonance in the nanocrystals approach values of some microseconds, which is typical for the type Ib diamond from which the nanoparticle is made. We conclude that despite the tiny size of these nanodiamonds the photoactive nitrogen-vacancy color centers retain their bulk properties to the benefit of numerous exciting potential applications in photonics, biomedical labeling, and imaging.

Nanoscale imaging magnetometry with diamond spins under ambient conditions.

Magnetic resonance imaging and optical microscopy are key technologies in the life sciences. For microbiological studies, especially of the inner workings of single cells, optical microscopy is normally used because it easily achieves resolution close to the optical wavelength. But in conventional microscopy, diffraction limits the resolution to about half the wavelength. Recently, it was shown that this limit can be partly overcome by nonlinear imaging techniques, but there is still a barrier to reaching the molecular scale. In contrast, in magnetic resonance imaging the spatial resolution is not determined by diffraction; rather, it is limited by magnetic field sensitivity, and so can in principle go well below the optical wavelength. The sensitivity of magnetic resonance imaging has recently been improved enough to image single cells, and magnetic resonance force microscopy has succeeded in detecting single electrons and small nuclear spin ensembles. However, this technique currently requires cryogenic temperatures, which limit most potential biological applications. Alternatively, single-electron spin states can be detected optically, even at room temperature in some systems. Here we show how magneto-optical spin detection can be used to determine the location of a spin associated with a single nitrogen-vacancy centre in diamond with nanometre resolution under ambient conditions. By placing these nitrogen-vacancy spins in functionalized diamond nanocrystals, biologically specific magnetofluorescent spin markers can be produced. Significantly, we show that this nanometre-scale resolution can be achieved without any probes located closer than typical cell dimensions. Furthermore, we demonstrate the use of a single diamond spin as a scanning probe magnetometer to map nanoscale magnetic field variations. The potential impact of single-spin imaging at room temperature is far-reaching. It could lead to the capability to probe biologically relevant spins in living cells.

Magnetic field diagnostics of plasmas based on coherent population trapping: theory and experiment.

We propose a local, all-optical method of magnetic field diagnostics for plasmas. This method is based on the phenomenon of coherent population trapping in a multilevel medium. The proposed technique allows one to detect both the strength and the orientation of the field. The feasibility of the method was tested in a proof-of-principle experiment in a low-pressure neon discharge.