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Pressure is a powerful thermodynamic parameter for tuning the magnetic properties of van der Waals magnets owing to their weak interlayer bonding. However, local magnetometry measurements under high pressure still remain elusive for this important class of emerging materials. Here we introduce a method enabling in situ magnetic imaging of van der Waals magnets under high pressure with sub-micron spatial resolution. Our approach relies on a quantum sensing platform based on boron-vacancy (V$_\text{B}^-$) centers in hexagonal boron nitride (hBN), which can be placed in atomic contact of any type of two-dimensional (2D) material within a van der Waals heterostructure. We first show that the V$_\text{B}^-$ center can be used as a magnetic field sensor up to pressures of a few GPa, a pressure range for which the properties of a wide variety of van der Waals magnets are efficiently altered. We then use V$_\text{B}^-$ centers in a thin hBN layer to perform magnetic imaging of a van der Waals magnet under pressure. As a proof of concept, we study the pressure-dependent magnetization in micrometer-sized flakes of $1T$-CrTe$_2$, whose evolution is explained by a shift of the Curie temperature. Besides providing a new path for studying pressure-induced phase transitions in van der Waals magnets, this work also opens up interesting perspectives for exploring the physics of 2D superconductors under pressure via local measurements of the Meissner effect., Comment: 10 pages, 5 figures

Defects in crystals can have a transformative effect on the properties and functionalities of solid-state systems. Dopants in semiconductors are core components in electronic and optoelectronic devices. The control of single color centers is at the basis of advanced applications for quantum technologies. Unintentional defects can also be detrimental to the crystalline structure and hinder the development of novel materials. Whatever the research perspective, the identification of defects is a key but complicated, and often long-standing issue. Here, we present a general methodology to identify point defects by combining isotope substitution and polytype control, with a systematic comparison between experiments and first-principles calculations. We apply this methodology to hexagonal boron nitride (hBN) and its ubiquitous color center emitting in the ultraviolet spectral range. From isotopic purification of the host hBN matrix, a local vibrational mode of the defect is uncovered, and isotope-selective carbon doping proves that this mode belongs to a carbon-based center. Then, by varying the stacking sequence of the host hBN matrix, we unveil different optical responses to hydrostatic pressure for the non-equivalent configurations of this ultraviolet color center. We conclude that this defect is a carbon dimer in the honeycomb lattice of hBN. Our results show that tuning the stacking sequence in different polytypes of a given crystal provides unique fingerprints contributing to the identification of defects in 2D materials.

The negatively-charged boron vacancy (V$_\text{B}^-$) center in hexagonal boron nitride (hBN) is currently garnering considerable attention for the design of two-dimensional (2D) quantum sensing units. Such developments require a precise understanding of the spin-dependent optical response of V$_\text{B}^-$ centers, which still remains poorly documented despite its key role for sensing applications. Here we investigate the spin-dependent photodynamics of V$_\text{B}^-$ centers in hBN by a series of time-resolved photoluminescence (PL) measurements. We first introduce a robust all-optical method to infer the spin-dependent lifetime of the excited states and the electron spin polarization of V$_\text{B}^-$ centers under optical pumping. Using these results, we then analyze PL time traces recorded at different optical excitation powers with a seven-level model of the V$_\text{B}^-$ center and we extract all the rates involved in the spin-dependent optical cycles, both under ambient conditions and at liquid helium temperature. These findings are finally used to study the impact of a vector magnetic field on the optical response. More precisely, we analyze PL quenching effects resulting from electron spin mixing induced by the magnetic field component perpendicular to the V$_\text{B}^-$ quantization axis. All experimental results are well reproduced by the seven-level model, illustrating its robustness to describe the spin-dependent photodymanics of V$_\text{B}^-$ centers. This work provides important insights into the properties of V$_\text{B}^-$ centers in hBN, which are valuable for future developments of 2D quantum sensing units., Comment: 11 pages, 9 figures

Ultrafast X-ray diffraction by the LCLS free-electron laser has been used to probe Charge Density Wave (CDW) systems under applied external currents. At sufficiently low currents, CDW wavefronts bend in the direction transverse to the 2k$_F$ wave vector. We show that this shear effect has the ability to focus or defocus hard X-ray beams, depending of the current direction, making it an electronic lens of a new kind, tunable at will from the Fraunhofer to the Fresnel regime. The effect is interpreted using the fractional Fourier transform showing how the macroscopic curvature of a nanometric modulation can be beneficially used to modify the propagation of X-ray beams., Comment: 3 pages, 3 figures

In this article, we review different studies based on advanced x-ray diffraction techniques - especially coherent x-ray diffraction - that allowed us to reveal the behaviour of such symmetry-breaking systems as Charge Density Wave (CDW) and Spin density Wave (SDW), through their local phase. After a brief introduction on the added value of using coherent x-rays, we show how the method can be applied to CDW and SDW systems, in both static and dynamical regimes. The approach allowed us to probe the particular sliding state of CDWs systems by observing them through their phase fluctuations, to which coherent x-rays are particularly sensitive. Several compounds stabilizing a CDW phase able to slide are presented, each with a different but clearly pronounced signature of the sliding state. Two main features emerge from this series of experiments which have been little treated until now, the influence of CDW pinning by the sample surfaces and the propagation of periodic phase defects such as charge solitons across the entire sample. Phase models describing the spatial and temporal properties of sliding CDWs are presented in the last part of this review., Comment: 41 pages, 20 figures

We report on electron spin resonance (ESR) spectroscopy of boron-vacancy (V$_\text{B}^-$) centers hosted in isotopically-engineered hexagonal boron nitride (hBN) crystals. We first show that isotopic purification of hBN with $^{15}$N yields a simplified and well-resolved hyperfine structure of V$_\text{B}^-$ centers, while purification with $^{10}$B leads to narrower ESR linewidths. These results establish isotopically-purified h$^{10}$B$^{15}$N crystals as the optimal host material for future use of V$_\text{B}^-$ spin defects in quantum technologies. Capitalizing on these findings, we then demonstrate optically-induced polarization of $^{15}$N nuclei in h$^{10}$B$^{15}$N, whose mechanism relies on electron-nuclear spin mixing in the V$_\text{B}^-$ ground state. This work opens up new prospects for future developments of spin-based quantum sensors and simulators on a two-dimensional material platform., Comment: 6 pages, 3 figure

The electronic orders appearing in condensed matter systems are originating from the precise arrangement of atoms constituting the crystal as well as their nature. This teneous relationship can lead to highly different phases in condensed matter, and drive electronic phase transitions. Here, we show that a very slight deformation of the crystal structure of TbTe$_3$ can have a dramatic influence on the electronic order that is stabilized. In particular, we show that the Charge Density Wave (CDW) developping along the $\vec{c}$ axis in the pristine state, switches to an orientation along $\vec{a}$ when the naturally orthorhombic system is turned into a tetragonal system. This is achieved by performing true biaxial mechanical deformation of a TbTe$_3$ sample from 250K to 375K, and by measuring both structural and electronic parameters with x-ray diffraction and transport measurements. We show that this switching transition is driven by the tetragonality parameter $a/c$, and that the transition occurs for $a=c$, with a coexistence region for $0.9985< a/c < 1.002$. The CDW transition temperature $T_c$ is found to have a linear dependence with $a/c$, with no saturation in the deformed states investigated here, while the gap saturates out of the coexistence region. The linear dependence of $T_c$ is accounted for within a tight-binding model. Our results question the relationship between the gap and $T_c$ in RTe$_3$ systems. More generally, our method of applying true biaxial deformation at cryogenic temperatures can be applied to many systems displaying electronic phase transitions, and opens a new route towards the study of coexisting or competing electronic orders in condensed matter.

The unique physical, mechanical, chemical, optical, and electronic properties of hexagonal boron nitride (hBN) make it a promising two-dimensional material for electronic, optoelectronic, nanophotonic, and quantum devices. Here we report on the changes in hBN's properties induced by isotopic purification in both boron and nitrogen. Previous studies on isotopically pure hBN have focused on purifying the boron isotope concentration in hBN from its natural concentration (approximately 20 at$\%$ $^{10}$B, 80 at$\%$ $^{11}$B) while using naturally abundant nitrogen (99.6 at$\%$ $^{14}$N, 0.4 at$\%$ $^{15}$N), i.e. almost pure $^{14}$N. In this study, we extend the class of isotopically-purified hBN crystals to $^{15}$N. Crystals in the four configurations, namely h$^{10}$B$^{14}$N, h$^{11}$B$^{14}$N, h$^{10}$B$^{15}$N, and h$^{11}$B$^{15}$N, were grown by the metal flux method using boron and nitrogen single isotope ($>99\%$) enriched sources, with nickel plus chromium as the solvent. In-depth Raman and photoluminescence spectroscopies demonstrate the high quality of the monoisotopic hBN crystals with vibrational and optical properties of the $^{15}$N-purified crystals at the state of the art of currently available $^{14}$N-purified hBN. The growth of high-quality h$^{10}$B$^{14}$N, h$^{11}$B$^{14}$N, h$^{10}$B$^{15}$N, and h$^{11}$B$^{15}$N opens exciting perspectives for thermal conductivity control in heat management, as well as for advanced functionalities in quantum technologies., Comment: 13 pages, 7 figures

Optically-active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this work, we first demonstrate that the electron spin resonance frequencies of boron vacancy centres (V$_\text{B}^-$) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of V$_\text{B}^-$ centres with the hBN thickness with a focus on (i) the zero-field splitting parameters, (ii) the optically-induced spin polarization rate and (iii) the longitudinal spin relaxation time. This work provides important insights into the properties of V$_\text{B}^-$ centres embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies., Comment: 7 pages, 3 figures

The boron-vacancy spin defect ($\text{V}_\text{B}^{-}$) in hexagonal boron nitride (hBN) has a great potential as a quantum sensor in a two-dimensional material that can directly probe various external perturbations in atomic-scale proximity to the quantum sensing layer. Here, we apply first principles calculations to determine the coupling of the $\text{V}_\text{B}^{-}$ electronic spin to strain and electric fields. Our work unravels the interplay between local piezoelectric and elastic effects contributing to the final response to the electric fields. The theoretical predictions are then used to analyse optically detected magnetic resonance (ODMR) spectra recorded on hBN crystals containing different densities of $\text{V}_\text{B}^{-}$ centres. We prove that the orthorhombic zero-field splitting parameter results from local electric fields produced by surrounding charge defects. By providing calculations of the spin-strain and spin-electric field couplings, this work paves the way towards applications of $\text{V}_\text{B}^{-}$ centres for quantitative electric field imaging and quantum sensing under pressure., Comment: 9 pages, 5 figures

We report successful incorporation of an ensemble of G centers in silicon-on-insulator (SOI) microrings using ion implantation and conventional nanofabrication. The coupling between the emitters and the resonant modes of the microrings is studied using continuous-wave and time-resolved microphotoluminescence (PL) experiments. We observe the resonant modes of the microrings on PL spectra, on the wide spectral range that is covered by G centers emission. By finely tuning the size of the microrings, we match their zero-phonon line at 1278 nm with a resonant mode of quality factor around 3000 and volume 7.2 (lambda over n)^3. The zero-phonon line intensity is enhanced by a factor of 5, both in continuous-wave and time-resolved measurements. This is attributed to the Purcell enhancement of zero-phonon spontaneous emission into the resonant mode and quantitatively understood considering the distribution of the G centers dipoles. Despite the enhancement of the zero-phonon emission, we do not observe any sizeable decrease of the average lifetime of the G centers, which points at a low radiative yield (<10%). We reveal the detrimental impact of parasitic defects in heavily implanted silicon, and discuss the perspectives for quantum electrodynamics experiments with individual color centers in lightly implanted SOI rings. Our results provide key information for the development of deterministic single photon sources for integrated quantum photonics., Comment: 24 pages, 7 figures, submitted to an international journal with peer review

Optically-active spin defects hosted in hexagonal boron nitride (hBN) are promising candidates for the development of a two-dimensional (2D) quantum sensing unit. Here, we demonstrate quantitative magnetic imaging with hBN flakes doped with negatively-charged boron-vacancy (V$_{\rm B}^-$) centers through neutron irradiation. As a proof-of-concept, we image the magnetic field produced by CrTe$_2$, a van der Waals ferromagnet with a Curie temperature slightly above $300$ K. Compared to other quantum sensors embedded in 3D materials, the advantages of the hBN-based magnetic sensor described in this work are its ease of use, high flexibility and, more importantly, its ability to be placed in close proximity to a target sample. Such a sensing unit will likely find numerous applications in 2D materials research by offering a simple way to probe the physics of van der Waals heterostructures., Comment: 5 pages, 3 figures, supplemental material as ancillary file

Spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of flexible two-dimensional quantum sensing platforms. Here we rely on hBN crystals isotopically enriched with either $^{10}$B or $^{11}$B to investigate the isotope-dependent properties of a spin defect featuring a broadband photoluminescence signal in the near infrared. By analyzing the hyperfine structure of the spin defect while changing the boron isotope, we first unambiguously confirm that it corresponds to the negatively-charged boron-vacancy center (${\rm V}_{\rm B}^-$). We then show that its spin coherence properties are slightly improved in $^{10}$B-enriched samples. This is supported by numerical simulations employing cluster correlation expansion methods, which reveal the importance of the hyperfine Fermi contact term for calculating the coherence time of point defects in hBN. Using cross-relaxation spectroscopy, we finally identify dark electron spin impurities as an additional source of decoherence. This work provides new insights into the properties of ${\rm V}_{\rm B}^-$ spin defects, which are valuable for the future development of hBN-based quantum sensing foils., Comment: 8 pages, 5 figures

The nitrogen-vacancy (NV) defect in diamond is an efficient quantum sensor of randomly fluctuating signals via relaxometry measurements. In particular, the longitudinal spin relaxation of the NV defect accelerates in the presence of magnetic noise with a spectral component at its electron spin resonance frequency. We look into this effect quantitatively by applying a calibrated and tunable magnetic noise on a single NV defect. We show that an increase of the longitudinal spin relaxation rate translates into a reduction of the photoluminescence (PL) signal emitted under continuous optical illumination, which can be explained using a simplified three-level model of the NV defect. This PL quenching mechanism offers a simple, all-optical method to detect magnetic noise sources at the nanoscale., Comment: 5 pages, 3 figures

We present a new realization of the textbook experiment consisting in single-photon interference based on the pulsed, optically excited photoluminescence of a single colour centre in a diamond nanocrystal. Interferences are created by wavefront-splitting with a Fresnel's biprism and observed by registering the "single-photon clicks" with an intensified CCD camera. This imaging detector provides also a real-time movie of the build-up of the single-photon fringes. We perform a second experiment with two detectors sensitive to photons that follow either one or the other interference path. Evidence for single photon behaviour is then obtained from the absence of time coincidence between detections in these two paths., Comment: Movie showing the built-up of interference fringes is available as a supplementary file

Studies of individual quantum systems, which have led to considerable progress in our understanding of quantum physics, have traditionally been associated with atomic gases. In the last decades however, the emphasis has shifted towards solid-state systems, which are much more practical for applications. In particular, a new field has recently emerged that is concerned with the study of quantum systems based on single spins localized near point defects in crystalline solids. One such system is the nitrogen-vacancy (NV) defect in diamond. Initially used as an experimental breadboard for testing concepts of quantum physics and quantum computation, the NV defect was soon proposed as a sensitive magnetometer, capable of detecting minute magnetic fields, down to ultimate level of single spins. This atomic-sized magnetometer can be used as a standalone sensor, or integrated into an imaging system providing spatial resolution down to the atomic scale. Diamond-based instruments thus offer new pathways to probe the magnetism of matter from the mesoscale down to the nanoscale. This book chapter gives an overview of the field of diamond-based magnetic sensing and imaging, with an emphasis on already demonstrated applications of this technology. The chapter is divided into three main sections. In Section 2, the underlying physics and methods of diamond-based magnetometry are described. Section 3 is devoted to various experimental implementations that employ this new class of sensors for magnetic sensing and imaging. Finally, some recent applications are presented in Section 4., Comment: 22 pages, 12 figure

While ferromagnets are at the heart of daily life applications, their large magnetization and resulting energy cost for switching bring into question their suitability for reliable low-power spintronic devices. Non-collinear antiferromagnetic systems do not suffer from this problem and often possess remarkable extra functionalities: non-collinear spin order may break space-inversion symmetry and thus allow electric-field control of magnetism, or produce emergent spin-orbit effects, which enable efficient spin-charge interconversion. To harness these unique traits for next-generation spintronics, the nanoscale control and imaging capabilities that are now routine for ferromagnets must be developed for antiferromagnetic systems. Here, using a non-invasive scanning nanomagnetometer based on a single nitrogen-vacancy (NV) defect in diamond, we demonstrate the first real-space visualization of non-collinear antiferromagnetic order in a magnetic thin film, at room temperature. We image the spin cycloid of a multiferroic BiFeO$_3$ thin film and extract a period of $\sim70$ nm, consistent with values determined by macroscopic diffraction. In addition, we take advantage of the magnetoelectric coupling present in BiFeO$_3$ to manipulate the cycloid propagation direction by an electric field. Besides highlighting the unique potential of NV magnetometry for imaging complex antiferromagnetic orders at the nanoscale, these results demonstrate how BiFeO$_3$ can be used as a versatile platform for the design of reconfigurable nanoscale spin textures.

Several efforts have been made to polarize the nearby nuclear environment of nitrogen vacancy (NV) centers for quantum metrology and quantum information applications. Different methods showed different nuclear spin polarization efficiencies and rely on electronic spin polarization associated to the NV center, which in turn crucially depends on the inter-system crossing. Recently, the rates involved in the inter-system crossing have been measured leading to different transition rate models. Here, we consider the effect of these rates on several nuclear polarization methods based on the level anti-crossing, and precession of the nuclear population while the electronic spin is in the ms = 0 and ms = 1 spin states. We show that the nuclear polarization depends on the power of optical excitation used to polarize the electronic spin. The degree of nuclear spin polarization is different for each transition rate model. Therefore, the results presented here are relevant for validating these models and for polarizing nuclear spins. Furthermore, we analyze the performance of each method by considering the nuclear position relative to the symmetry axis of the NV center., Comment: 12 pages, 6 figures + 7 pages supplementary, comments are welcome

We demonstrate room-temperature ferromagnetism with in-plane magnetic anisotropy in thin flakes of the CrTe$_2$ van der Waals ferromagnet. Using quantitative magnetic imaging with a single spin magnetometer based on a nitrogen-vacancy defect in diamond, we infer a room-temperature in-plane magnetization in the range of $M\sim 27$ kA/m for flakes with thicknesses down to $20$ nm. In addition, our measurements indicate that the orientation of the magnetization is not determined solely by shape anisotropy in micron-sized CrTe$_2$ flakes, which suggest the existence of a non-negligible magnetocrystalline anisotropy. These results make CrTe$_2$ a unique system in the growing family of van der Waals ferromagnets, as it is the only material platform known to date which offers an intrinsic in-plane magnetization and a Curie temperature above $300$ K in thin flakes., Comment: 9 pages, 5 figures

We report the detection of individual emitters in silicon belonging to seven different families of optically-active point defects. These fluorescent centers are created by carbon implantation of a commercial silicon-on-insulator wafer usually employed for integrated photonics. Single photon emission is demonstrated over the [1.1,1.55]-$\mu$m range, spanning the O- and C-telecom bands. We analyse their photoluminescence spectrum, dipolar emission and optical relaxation dynamics at 10K. For a specific family, we show a constant emission intensity at saturation from 10K to temperatures well above the 77K-liquid nitrogen temperature. Given the advanced control over nanofabrication and integration in silicon, these novel artificial atoms are promising candidates for Si-based quantum technologies.

A Charge Density Wave (CDW) submitted to an electric field displays a strong shear deformation because of pinning at the lateral surfaces of the sample. This CDW transverse pinning was recently observed but has received little attention from a theoretical point of view until now despite important consequences on electrical conductivity properties. Here, we provide a description of this phenomenon by considering a CDW submitted to an external dc electric field and constrained by boundary conditions including both longitudinal pinning due to electrical contacts and transverse surface pinning. A simple formula for the CDW phase is obtained in 3D by using the Green function and image charges method. In addition, an analytical expression of the threshold field dependence on both length and sample cross section is obtained by considering the phase slip process. We show that the experimental data are well reproduced with this model and that bulk pinning can be neglected. This study shows that the dynamical properties of CDW systems could be mainly driven by boundary effects, despite the comparatively huge sample volumes., Comment: 7 pages of main text, 7 pages of appendices 15 figures

Nitrogen-Vacancy centers in diamond possess an electronic spin resonance that strongly depends on temperature, which makes them efficient temperature sensor with a sensitivity down to a few mK/$\sqrt{\rm Hz}$. However, the high thermal conductivity of the host diamond may strongly damp any temperature variations, leading to invasive measurements when probing local temperature distributions. In view of determining possible and optimal configurations for diamond-based wide-field thermal imaging, we here investigate, both experimentally and numerically, the effect of the presence of diamond on microscale temperature distributions. Three geometrical configurations are studied: a bulk diamond substrate, a thin diamond layer bonded on quartz and diamond nanoparticles dispersed on quartz. We show that the use of bulk diamond substrates for thermal imaging is highly invasive, in the sense that it prevents any substantial temperature increase. Conversely, thin diamond layers partly solve this issue and could provide a possible alternative for microscale thermal imaging. Dispersions of diamond nanoparticles throughout the sample appear as the most relevant approach as they do not affect the temperature distribution, although NV centers in nanodiamonds yield lower temperature sensitivities compared to bulk diamond., Comment: 5 pages, 3 figures

Given its unrivaled potential of integration and scalability, silicon is likely to become a key platform for large-scale quantum technologies. Individual electron-encoded artificial atoms either formed by impurities or quantum dots have emerged as a promising solution for silicon-based integrated quantum circuits. However, single qubits featuring an optical interface needed for large-distance exchange of information have not yet been isolated in such a prevailing semiconductor. Here we show the isolation of single optically-active point defects in a commercial silicon-on-insulator wafer implanted with carbon atoms. These artificial atoms exhibit a bright, linearly polarized single-photon emission at telecom wavelengths suitable for long-distance propagation in optical fibers. Our results demonstrate that despite its small bandgap (~ 1.1 eV) a priori unfavorable towards such observation, silicon can accommodate point defects optically isolable at single scale, like in wide-bandgap semiconductors. This work opens numerous perspectives for silicon-based quantum technologies, from integrated quantum photonics to quantum communications and metrology.

We demonstrate that magnetic skyrmions with a mean diameter around 60 nm can be stabilized at room temperature and zero external magnetic field in an exchange-biased Pt/Co/NiFe/IrMn multilayer stack. This is achieved through an advanced optimization of the multilayer stack composition in order to balance the different magnetic energies controlling the skyrmion size and stability. Magnetic imaging is performed both with magnetic force microscopy and scanning Nitrogen-Vacancy magnetometry, the latter providing unambiguous measurements at zero external magnetic field. In such samples, we show that exchange bias provides an immunity of the skyrmion spin texture to moderate external magnetic field, in the tens of mT range, which is an important feature for applications as memory devices. These results establish exchange-biased multilayer stacks as a promising platform towards the effective realization of memory and logic devices based on magnetic skyrmions., Comment: 5 pages, 3 figures

Antiferromagnetic thin films are currently generating considerable excitement for low dissipation magnonics and spintronics. However, while tuneable antiferromagnetic textures form the backbone of functional devices, they are virtually unknown at the submicron scale. Here we image a wide variety of antiferromagnetic spin textures in multiferroic BiFeO3 thin films that can be tuned by strain and manipulated by electric fields through room temperature magnetoelectric coupling. Using piezoresponse force microscopy and scanning NV magnetometry in self-organized ferroelectric patterns of BiFeO3, we reveal how strain stabilizes different types of non-collinear antiferromagnetic states (bulk-like and exotic spin cycloids) as well as collinear antiferromagnetic textures. Beyond these local-scale observations, resonant elastic X-ray scattering confirms the existence of both types of spin cycloids. Finally, we show that electric-field control of the ferroelectric landscape induces transitions either between collinear and non-collinear states or between different cycloids, offering perspectives for the design of reconfigurable antiferromagnetic spin textures on demand.

Diamond is a host for a wide variety of colour centres that have demonstrated outstanding optical and spin properties. Among them, the nitrogen-vacancy (NV) centre is by far the most investigated owing to its superior characteristics, which promise the development of highly sophisticated quantum devices, in particular for sensing applications. Nevertheless, harnessing the potential of these centres mainly relies on the availability of high quality and purity diamond single crystals that need to be specially designed and engineered for this purpose. The plasma assisted Chemical Vapour Deposition (CVD) has become a key enabling technology in this field of research. Nitrogen can indeed be directly in-situ doped into a high crystalline quality diamond matrix in a controlled way allowing the production of single isolated centres or ensembles that can potentially be integrated into a device. In this paper we will provide an overview on the requirements for synthesizing quantum-grade diamond films by CVD. These include the reduction of impurities and surrounding spins that limit coherence times, the control of NV density in a wide range of concentrations as well as their spatial localization within the diamond. Enhancing the charge state and preferential orientation of the colour centres is also discussed. These improvements in material fabrication have contributed to position diamond as one of the most promising solid-state quantum system and the first industrial applications in sensing are just starting to emerge., Comment: Review paper, 41 pages, 17 figures

Incommensurate charge density waves (CDW) have the extraordinary ability to display non-Ohmic behavior when submitted to an external field. The mechanism leading to this non trivial dynamics is still not well understood, although recent experimental studies tend to prove that it is due to solitonic transport. Solitons could come from the relaxation of the strained CDW within an elastic-to-plastic transition. However, the nucleation process and the transport of these charged topological objects have never been observed at the local scale until now. In this letter, we use in-situ scanning x-ray micro-diffraction with micrometer resolution of a NbSe$_3$ sample designed to have sliding and non-sliding areas. Direct imaging of the charge density wave deformation is obtained using an analytical approach based on the phase gradient to disentangle the transverse from the longitudinal components over a large surface of a hundred microns size. We show that the CDW dissociates itself from the host lattice in the sliding regime and displays a large transverse deformation, ten times larger than the longitudinal one and strongly dependent on the amplitude and the direction of the applied currents. This deformation continuously extends across the macroscopic sample dimensions, over a distance 10 000 times greater than the CDW wavelength despite the presence of strong defects while remaining strongly pinned by the lateral surfaces. This 2D quantitative study highlights the prominent role of shear effect that should play a significant role in the nucleation of solitons.

We demonstrate room-temperature stabilization of dipolar magnetic skyrmions with diameters in the range of $100$ nm in a single ultrathin layer of the Heusler alloy Co$_2$FeAl (CFA) under moderate magnetic fields. Current-induced skyrmion dynamics in microwires is studied with a scanning Nitrogen-Vacancy magnetometer operating in the photoluminescence quenching mode. We first demonstrate skyrmion nucleation by spin-orbit torque and show that its efficiency can be significantly improved using tilted magnetic fields, an effect which is not specific to Heusler alloys and could be advantageous for future skyrmion-based devices. We then show that current-induced skyrmion motion remains limited by strong pinning effects, even though CFA is a magnetic material with a low magnetic damping parameter., Comment: 5 pages, 4 figures

Control of the crystalline orientation of nitrogen-vacancy (NV) defects in diamond is here demonstrated by tuning the temperature of chemical vapor deposition (CVD) growth on a (113)-oriented diamond substrate. We show that preferential alignment of NV defects along the [111] axis is significantly improved when the CVD growth temperature is decreased. This effect is then combined with temperature-dependent incorporation of NV defects during the CVD growth to obtain preferential alignment over dense ensembles of NV defects spatially localized in thin diamond layers. These results demonstrate that growth temperature can be exploited as an additional degree of freedom to engineer optimized diamond samples for quantum sensing applications., Comment: 6 pages, 3 figures

We analyze the properties of a pulsed Coherent Population Trapping protocol that uses a controlled decay from the excited state in a $\Lambda$-level scheme. We study this problem analytically and numerically and find regimes where narrow transmission, absorption, or fluorescence spectral lines occur. We then look for optimal frequency measurements using these spectral features by computing the Allan deviation in the presence of ground state decoherence and show that the protocol is on a par with Ramsey-CPT. We discuss possible implementations with ensembles of alkali atoms and single ions and demonstrate that typical pulsed-CPT experiments that are realized on femto-second time-scales can be implemented on micro-seconds time-scales using this scheme., Comment: 9 pages, 7 figures

Nitrogen-vacancy magnetic microscopy is employed in quenching mode as a non-invasive, high resolution tool to investigate the morphology of isolated skyrmions in ultrathin magnetic films. The skyrmion size and shape are found to be strongly affected by local pinning effects and magnetic field history. Micromagnetic simulations including static disorder, based on a physical model of grain-to-grain thickness variations, reproduce all experimental observations and reveal the key role of disorder and magnetic history in the stabilization of skyrmions in ultrathin magnetic films. This work opens the way to an in-depth understanding of skyrmion dynamics in real, disordered media., Comment: 9 pages, 8 figures, including supplementary informations

We addressed the carrier dynamics in so-called G-centers in silicon (consisting of substitutional-interstitial carbon pairs interacting with interstitial silicons) obtained via ion implantation into a silicon-on-insulator wafer. For this point defect in silicon emitting in the telecommunication wavelength range, we unravel the recombination dynamics by time-resolved photoluminescence spectroscopy. More specifically, we performed detailed photoluminescence experiments as a function of excitation energy, incident power, irradiation fluence and temperature in order to study the impact of radiative and non-radiative recombination channels on the spectrum, yield and lifetime of G-centers. The sharp line emitting at 969 meV ($\sim$1280 nm) and the broad asymmetric sideband developing at lower energy share the same recombination dynamics as shown by time-resolved experiments performed selectively on each spectral component. This feature accounts for the common origin of the two emission bands which are unambiguously attributed to the zero-phonon line and to the corresponding phonon sideband. In the framework of the Huang-Rhys theory with non-perturbative calculations, we reach an estimation of 1.6$\pm$0.1 $\angstrom$ for the spatial extension of the electronic wave function in the G-center. The radiative recombination time measured at low temperature lies in the 6 ns-range. The estimation of both radiative and non-radiative recombination rates as a function of temperature further demonstrate a constant radiative lifetime. Finally, although G-centers are shallow levels in silicon, we find a value of the Debye-Waller factor comparable to deep levels in wide-bandgap materials. Our results point out the potential of G-centers as a solid-state light source to be integrated into opto-electronic devices within a common silicon platform.

Femtosecond time-resolved X-ray diffraction is used to study a photo-induced phase transition between two charge density wave (CDW) states in 1T-TaS$_2$, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photo-induced I-CDW phase then develops through a nucleation/growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a non-conservative order parameter., Comment: 6 pages, 5 figures

We report here on time-resolved x-ray diffraction measurements following femtosecond laser excitation in pure bulk chromium. Comparing the evolution of incommensurate charge-density-wave (CDW) and atomic lattice reflections, we show that, few nanoseconds after laser excitation, the CDW undergoes different structural changes than the atomic lattice. We give evidence for a transient CDW shear strain that breaks the lattice point symmetry. This strain is characteristic of sliding CDWs, as observed in other incommensurate CDW systems, suggesting the laser-induced CDW sliding capability in 3D systems. This first evidence opens perspectives for unconventional laser-assisted transport of correlated charges., Comment: 4 pages with 4 figures + supplemental material with 4 figures, Published in Phys. Rev. Lett. 2016

The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. Here we present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V2O3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A1g coherent phonon. This configuration is in stark contrast with the thermally accessible ones - the A1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned., Comment: 6 pages, 4 figures

Among a variety of layered materials used as building blocks in van der Waals heterostructures, hexagonal boron nitride (hBN) appears as an ideal platform for hosting optically-active defects owing to its large bandgap ($\sim 6$ eV). Here we study the optical response of a high-purity hBN crystal under green laser illumination. By means of photon correlation measurements, we identify individual defects emitting a highly photostable fluorescence under ambient conditions. A detailed analysis of the photophysical properties reveals a high quantum efficiency of the radiative transition, leading to a single photon source with very high brightness. These results illustrate how the wide range of applications offered by hBN could be further extended to photonic-based quantum information science and metrology., Comment: 5 pages, 4 figures

Solitons are peculiar excitations that appear in a wide range of nonlinear systems such as in fluids or optics. We show here that the collective transport of charges observed in charge density wave (CDW) systems can be explained by using a similar theory based on a traveling soliton lattice. Coherent x-ray diffraction experiment performed in the sliding state of a CDW material reveals peculiar diffraction patterns in good agreement with this assumption. Therefore, the collective transport of charges in CDW systems may be due to a nonlinear interaction leading to a self-localized excitation, carrying charges without deformation through the sample, on top of the CDW ground state. This single theory explains why charges remain spatially correlated over very long distances and reconciles the main features of sliding CDW systems, either observed by transport measurements or diffraction., Comment: 3 pages, 3 figures

The Dzyaloshinskii-Moriya Interaction (DMI) has recently attracted considerable interest owing to its fundamental role in the stabilization of chiral spin textures in ultrathin ferromagnets, which are interesting candidates for future spintronic technologies. Here we employ a scanning nano-magnetometer based on a single nitrogen-vacancy (NV) defect in diamond to locally probe the strength of the interfacial DMI in CoFeB/MgO ultrathin films grown on different heavy metal underlayers X=Ta,TaN, and W. By measuring the stray field emanating from DWs in micron-long wires of such materials, we observe deviations from the Bloch profile for TaN and W underlayers that are consistent with a positive DMI value favoring right-handed chiral spin structures. Moreover, our measurements suggest that the DMI constant might vary locally within a single sample, illustrating the importance of local probes for the study of magnetic order at the nanoscale., Comment: 9 pages, 4 figures

We report on sliding Charge Density Wave (CDW) in the quasi two-dimensional TbTe$_3$ system probed by coherent x-ray diffraction combined with {\it in-situ} transport measurements. We show that the non-Ohmic conductivity in TbTe$_3$ is made possible thanks to a strong distortion of the CDW. Our diffraction experiment versus current shows first that the CDW remains undeformed below the threshold current I$_S$ and then suddenly rotates and reorders by motion above threshold. Contrary to quasi-one dimensional systems, the CDW in TbTe$_3$ does not display any phase shifts below I$_S$ and tolerates only slow spatial variations of the phase above. This is a first observation of CDW behavior in the bulk in a quasi-two dimensional system allowing collective transport of charges at room temperature., Comment: submitted to PRB

We analyze the impact of electric field and magnetic field fluctuations in the decoherence of the electronic spin associated with a single nitrogen-vacancy (NV) defect in diamond by engineering spin eigenstates protected either against magnetic noise or against electric noise. The competition between these noise sources is analyzed quantitatively by changing their relative strength through modifications of the environment. This study provides significant insights into the decoherence of the NV electronic spin, which is valuable for quantum metrology and sensing applications., Comment: 8 pages, 4 figures, including supplementary informations

This article reviews efforts to build a new type of quantum device, which combines an ensemble of electronic spins with long coherence times, and a small-scale superconducting quantum processor. The goal is to store over long times arbitrary qubit states in orthogonal collective modes of the spin-ensemble, and to retrieve them on-demand. We first present the protocol devised for such a multi-mode quantum memory. We then describe a series of experimental results using NV center spins in diamond, which demonstrate its main building blocks: the transfer of arbitrary quantum states from a qubit into the spin ensemble, and the multi-mode retrieval of classical microwave pulses down to the single-photon level with a Hahn-echo like sequence. A reset of the spin memory is implemented in-between two successive sequences using optical repumping of the spins., Comment: 27 pages, 7 figures

Coherent control of quantum systems has far-reaching implications in quantum engineering. In this context, coherent population trapping (CPT) involving dark resonances has played a prominent role, leading to a wealth of major applications including laser cooling of atoms and molecules, optical magnetometry, light storage and highly precise atomic clocks. Extending CPT methods to individual solid-state quantum systems has been only achieved in cryogenic environments for electron spin impurities and superconducting circuits. Here, we demonstrate efficient CPT of a single nuclear spin in a room temperature solid. To this end, we make use of a three-level system with a $\Lambda$-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. Dark state pumping requires a relaxation mechanism which, in atomic systems, is simply provided by spontaneous emission. In this work, the relaxation process is externally controlled through incoherent optical pumping and separated in time from consecutive coherent microwave excitations of the nuclear spin $\Lambda$-system. Such a pumping scheme with controlled relaxation allows us (i) to monitor the sequential accumulation of population into the dark state and (ii) to reach a new regime of CPT dynamics for which periodic arrays of dark resonances can be observed, owing to multiple constructive interferences. This work offers new prospects for quantum state preparation, information storage in hybrid quantum systems and metrology., Comment: 13 pages including supplementary information, links to figures corrected

We present an experimental and theoretical study exploring surface effects on the evolution of the metal-insulator transition in the model Mott-Hubbard compound Cr-doped V$_2$O$_3$. We find a microscopic domain formation that is clearly affected by the surface crystallographic orientation. Using scanning photoelectron microscopy and X-ray diffraction, we find that surface defects act as nucleation centers for the formation of domains at the temperature-induced isostructural transition and favor the formation of microscopic metallic regions. A density functional theory plus dynamical mean field theory study of different surface terminations shows that the surface reconstruction with excess vanadyl cations leads to doped, and hence more metallic surface states, explaining our experimental observations., Comment: 5 pages, 4 figures

We report the storage of microwave pulses at the single-photon level in a spin-ensemble memory consisting of $10^{10}$ NV centers in a diamond crystal coupled to a superconducting LC resonator. The energy of the signal, retrieved $100\, \mu \mathrm{s}$ later by spin-echo techniques, reaches $0.3\%$ of the energy absorbed by the spins, and this storage efficiency is quantitatively accounted for by simulations. This figure of merit is sufficient to envision first implementations of a quantum memory for superconducting qubits., Comment: 6 pages

Thick CVD diamond layers were successfully grown on (113)-oriented substrates. They exhibited smooth surface morphologies and a crystalline quality comparable to (100) electronic grade material, and much better than (111)-grown layers. High growth rates (15-50 {\mu}m/h) were obtained while nitrogen doping could be achieved in a fairly wide range without seriously imparting crystalline quality. Electron spin resonance measurements were carried out to determine NV centers orientation and concluded that one specific orientation has an occurrence probability of 73 % when (100)-grown layers show an equal distribution in the 4 possible directions. A spin coherence time of around 270 {\mu}s was measured which is equivalent to that reported for material with similar isotopic purity. Although a higher degree of preferential orientation was achieved with (111)-grown layers (almost 100 %), the ease of growth and post-processing of the (113) orientation make it a potentially useful material for magnetometry or other quantum mechanical applications., Comment: 15 pages, 6 figures

We present a new approach to infer the surface density of magnetic moments $I_s$ in ultrathin ferromagnetic films with perpendicular anisotropy. It relies on quantitative stray field measurements with an atomic-size magnetometer based on the nitrogen-vacancy center in diamond. The method is applied to microstructures patterned in a 1-nm-thick film of CoFeB. We report measurements of $I_s$ with a few percent uncertainty and a spatial resolution in the range of $(100$ nm)$^2$, an improvement by several orders of magnitude over existing methods. As an example of application, we measure the modifications of $I_s$ induced by local irradiation with He$^+$ ions in an ultrathin ferromagnetic wire. This method offers a new route to study variations of magnetic properties at the nanoscale., Comment: 9 pages and 7 figures including main text and Supplemental Information

The recent observation of current-induced domain wall (DW) motion with large velocity in ultrathin magnetic wires has opened new opportunities for spintronic devices. However, there is still no consensus on the underlying mechanisms of DW motion. Key to this debate is the DW structure, which can be of Bloch or N\'eel type, and dramatically affects the efficiency of the different proposed mechanisms. To date, most experiments aiming to address this question have relied on deducing the DW structure and chirality from its motion under additional in-plane applied fields, which is indirect and involves strong assumptions on its dynamics. Here we introduce a general method enabling direct, in situ, determination of the DW structure in ultrathin ferromagnets. It relies on local measurements of the stray field distribution above the DW using a scanning nanomagnetometer based on the Nitrogen-Vacancy defect in diamond. We first apply the method to a Ta/Co40Fe40B20(1 nm)/MgO magnetic wire and find clear signature of pure Bloch DWs. In contrast, we observe left-handed N\'eel DWs in a Pt/Co(0.6 nm)/AlOx wire, providing direct evidence for the presence of a sizable Dzyaloshinskii-Moriya interaction (DMI) at the Pt/Co interface. This method offers a new path for exploring interfacial DMI in ultrathin ferromagnets and elucidating the physics of DW motion under current., Comment: Main text and Supplementary Information, 33 pages and 12 figures