Coherent Population Trapping of a Single Nuclear Spin Under Ambient Conditions.

We demonstrate coherent population trapping of a single nuclear spin in a room-temperature solid. To this end, we exploit a three-level system with a Λ configuration in the microwave domain, which consists of nuclear spin states addressed through their hyperfine coupling to the electron spin of a single nitrogen-vacancy defect in diamond. Moreover, the Λ-scheme relaxation is externally controlled through incoherent optical pumping and separated in time from consecutive coherent microwave excitations. Such a scheme allows us (i) to monitor the sequential accumulation of population into the dark state and (ii) to reach a novel regime of coherent population trapping dynamics for which periodic arrays of dark resonances can be observed, owing to multiple constructive interferences. This Letter offers new prospects for quantum state preparation, information storage in hybrid quantum systems, and metrology.

Magnetometry with nitrogen-vacancy defects in diamond.

The isolated electronic spin system of the nitrogen-vacancy (NV) centre in diamond offers unique possibilities to be employed as a nanoscale sensor for detection and imaging of weak magnetic fields. Magnetic imaging with nanometric resolution and field detection capabilities in the nanotesla range are enabled by the atomic-size and exceptionally long spin-coherence times of this naturally occurring defect. The exciting perspectives that ensue from these characteristics have triggered vivid experimental activities in the emerging field of 'NV magnetometry'. It is the purpose of this article to review the recent progress in high-sensitivity nanoscale NV magnetometry, generate an overview of the most pertinent results of the last years and highlight perspectives for future developments. We will present the physical principles that allow for magnetic field detection with NV centres and discuss first applications of NV magnetometers that have been demonstrated in the context of nano magnetism, mesoscopic physics and the life sciences.

Probing the dynamics of a nuclear spin bath in diamond through time-resolved central spin magnetometry.

Using fast electron spin resonance spectroscopy of a single nitrogen-vacancy defect in diamond, we demonstrate real-time readout of the Overhauser field produced by its nuclear spin environment under ambient conditions. These measurements enable narrowing the Overhauser field distribution by postselection, corresponding to a conditional preparation of the nuclear spin bath. Correlations of the Overhauser field fluctuations are quantitatively inferred by analyzing the Allan deviation over consecutive measurements. This method allows us to extract the dynamics of weakly coupled nuclear spins of the reservoir.

Single-shot readout of multiple nuclear spin qubits in diamond under ambient conditions.

We use the electronic spin of a single nitrogen-vacancy defect in diamond to observe the real-time evolution of neighboring single nuclear spins under ambient conditions. Using a diamond sample with a natural abundance of (13)C isotopes, we first demonstrate high fidelity initialization and single-shot readout of an individual (13)C nuclear spin. By including the intrinsic (14)N nuclear spin of the nitrogen-vacancy defect in the quantum register, we then report the simultaneous observation of quantum jumps linked to both nuclear spin species, providing an efficient initialization of the two qubits. These results open up new avenues for diamond-based quantum information processing including active feedback in quantum error correction protocols and tests of quantum correlations with solid-state single spins at room temperature.

Second-harmonic generation from coupled plasmon modes in a single dimer of gold nanospheres.

We show that a dimer made of two gold nanospheres exhibits a remarkable efficiency for second-harmonic generation under femtosecond optical excitation. The detectable nonlinear emission for the given particle size and excitation wavelength arises when the two nanoparticles are as close as possible to contact, as in situ controlled and measured using the tip of an atomic force microscope. The excitation wavelength dependence of the second-harmonic signal supports a coupled plasmon resonance origin with radiation from the dimer gap. This nanometer-size light source might be used for high-resolution near-field optical microscopy.

Hybrid quantum circuit with a superconducting qubit coupled to a spin ensemble.

We report the experimental realization of a hybrid quantum circuit combining a superconducting qubit and an ensemble of electronic spins. The qubit, of the transmon type, is coherently coupled to the spin ensemble consisting of nitrogen-vacancy centers in a diamond crystal via a frequency-tunable superconducting resonator acting as a quantum bus. Using this circuit, we prepare a superposition of the qubit states that we store into collective excitations of the spin ensemble and retrieve back into the qubit later on. These results constitute a proof of concept of spin-ensemble based quantum memory for superconducting qubits.

Strong coupling of a spin ensemble to a superconducting resonator.

We report the realization of a quantum circuit in which an ensemble of electronic spins is coupled to a frequency tunable superconducting resonator. The spins are nitrogen-vacancy centers in a diamond crystal. The achievement of strong coupling is manifested by the appearance of a vacuum Rabi splitting in the transmission spectrum of the resonator when its frequency is tuned through the nitrogen-vacancy center electron spin resonance.

Defocused imaging of second harmonic generation from a single nanocrystal.

We demonstrate the direct imaging of the second harmonic generation radiation from a single nonlinear nanocrystal using defocused nonlinear microscopy. This technique allows the retrieval of complete information on the 3D orientation of a nanocrystal as well as possible deviations from its purely crystalline nature, in a simple experimental implementation. The obtained images are modeled by calculation of the radiation diagram from a nonlinear dipole that accounts for the excitation beam, the crystal symmetry and the particle size. Experimental demonstrations are performed on Potassium Titanyl Phosphase (KTP) nanocrystals. The shape and structure of the radiation images show a strong dependence on both crystal orientation and field polarization state, as expected by the specific nonlinear coherent coupling between the induced dipole and the excitation field polarization state.

The nature of domain walls in ultrathin ferromagnets revealed by scanning nanomagnetometry.

The capacity to propagate magnetic domain walls with spin-polarized currents underpins several schemes for information storage and processing using spintronic devices. A key question involves the internal structure of the domain walls, which governs their response to certain current-driven torques such as the spin Hall effect. Here we show that magnetic microscopy based on a single nitrogen-vacancy defect in diamond can provide a direct determination of the internal wall structure in ultrathin ferromagnetic films under ambient conditions. We find pure Bloch walls in Ta/CoFeB(1 nm)/MgO, while left-handed Néel walls are observed in Pt/Co(0.6 nm)/AlOx. The latter indicates the presence of a sizable interfacial Dzyaloshinskii-Moriya interaction, which has strong bearing on the feasibility of exploiting novel chiral states such as skyrmions for information technologies.

Nanoscale imaging and control of domain-wall hopping with a nitrogen-vacancy center microscope.

The control of domain walls in magnetic wires underpins an emerging class of spintronic devices. Propagation of these walls in imperfect media requires defects that pin them to be characterized on the nanoscale. Using a magnetic microscope based on a single nitrogen-vacancy (NV) center in diamond, we report domain-wall imaging on a 1-nanometer-thick ferromagnetic nanowire and directly observe Barkhausen jumps between two pinning sites spaced 50 nanometers apart. We further demonstrate in situ laser control of these jumps, which allows us to drag the domain wall along the wire and map the pinning landscape. Our work demonstrates the potential of NV microscopy to study magnetic nano-objects in complex media, whereas controlling domain walls with laser light may find an application in spintronic devices.

Stray-field imaging of magnetic vortices with a single diamond spin.

Despite decades of advances in magnetic imaging, obtaining direct, quantitative information with nanometre scale spatial resolution remains an outstanding challenge. Recently, a technique has emerged that employs a single nitrogen-vacancy defect in diamond as an atomic-size magnetometer, which promises significant advances. However, the effectiveness of the technique when applied to magnetic nanostructures remains to be demonstrated. Here we use a scanning nitrogen-vacancy magnetometer to image a magnetic vortex, which is one of the most iconic objects of nanomagnetism, owing to the small size (~10 nm) of the vortex core. We report three-dimensional, vectorial and quantitative measurements of the stray magnetic field emitted by a vortex in a ferromagnetic square dot, including the detection of the vortex core. We find excellent agreement with micromagnetic simulations, both for regular vortex structures and for higher-order magnetization states. These experiments establish scanning nitrogen-vacancy magnetometry as a practical and unique tool for fundamental studies in nanomagnetism.

Photon antibunching in the fluorescence of a single dye molecule embedded in a thin polymer film.

We used scanning confocal microscopy to study the fluorescence from a single terrylene molecule embedded in a thin polymer film of polymethyl methacrylate, at room temperature, with a high signal-to-background ratio. The photon-pair correlation function g((2))(tau) exhibits perfect photon antibunching at tau = 0 and a limit of 1.3, compatible with bunching associated with the molecular triplet state. Application of this molecular system to a triggered single-photon source based on single-molecule fluorescence is investigated.

Direct measurement of the photon statistics of a triggered single photon source.

We studied intensity fluctuations of a single photon source relying on the pulsed excitation of the fluorescence of a single molecule at room temperature. We directly measured the Mandel parameter Q(T) over 4 orders of magnitude of observation time scale T by recording every photocount. On time scale of a few excitation periods, sub-Poissonian statistics is clearly observed and the probablility of two-photons events is 10 times smaller than Poissonian pulses. On longer times, blinking in the fluorescence, due to the molecular triplet state, produces an excess of noise.