arXiv subjects

V. Jacques

Publications and source records attributed to V. Jacques.

At least 19 recordsLinked to original sources

arXiv2025

Spin defects in hexagonal boron nitride as two-dimensional strain sensors

Lattice deformation is a powerful way to engineer the properties of two-dimensional (2D) materials, making their precise measurement an important challenge for both fundamental science and technological applications. Here, we demonstrate that boron-vacancy (V$_\text{B}^-$) color centers in hexagonal boron nitride (hBN) enable quantitative strain sensing with sub-micrometer spatial resolution. Using this approach, we precisely quantify the strain-induced shift of the E$_{\rm 2g}$ Raman mode in a multilayer hBN flake under uniaxial stress, establishing V$_\text{B}^-$ centers as a new tool for strain metrology in van der Waals heterostructures. Beyond strain sensing, our work also highlights the unique multimodal sensing functionalities offered by V$_\text{B}^-$ centers, which will be valuable for future studies of strain-engineered 2D materials.

cond-mat.mtrl-sci↗

arXiv2025

Growth of rhombohedral boron nitride crystals using an iron flux

We report the growth of high quality rhombohedral boron nitride (rBN) crystals by the iron flux method at atmospheric pressure. In contrast to the lamellar structure of standard hexagonal boron nitride (hBN) covering the metal ingot, the current synthetized BN shell is composed of many triangular bulk crystallites, of submillimeter size, predominantly in the rhombohedral phase, with only weak traces of hBN detected by high resolution X-ray diffraction. The low-temperature photoluminescence emission confirms the excellent quality of the rhombohedral stacking with unprecedented width for all phonon replicas at the band edge. The Raman spectra are characterized by the absence of any low-energy modes at $\sim50$ cm$^{-1}$, the presence of an extended band around $800$ cm$^{-1}$ and an asymmetric high energy mode at $1366$ cm$^{-1}$. These observations are in very good agreement with the phonon dispersion calculated for the rhombohedral primitive cell with $C_{3v}$ symmetry.

cond-mat.mtrl-sci↗

arXiv2025

Magnetic imaging under high pressure with a spin-based quantum sensor integrated in a van der Waals heterostructure

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.

cond-mat.mtrl-sci↗

arXiv2024

Isotope substitution and polytype control for point defects identification: the case of the ultraviolet color center in hexagonal boron nitride

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.

cond-mat.mtrl-sci↗

arXiv2024

Spin-dependent photodynamics of boron-vacancy centers in hexagonal boron nitride

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.

cond-mat.mtrl-sci↗

arXiv2023

Isotopic control of the boron-vacancy spin defect in hexagonal boron nitride

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.

quant-ph↗

arXiv2023

Boron and nitrogen isotope effects on hexagonal boron nitride properties

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.

cond-mat.mtrl-sci↗

arXiv2023

Optically-active spin defects in few-layer thick hexagonal boron nitride

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.

quant-ph↗

arXiv2023

A planar defect spin sensor in a two-dimensional material susceptible to strain and electric fields

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.

quant-ph↗

arXiv2022

Cavity-enhanced zero-phonon emission from an ensemble of G centers in a silicon-on-insulator microring

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.

physics.optics↗

arXiv2022

Magnetic imaging with spin defects in hexagonal boron nitride

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.

cond-mat.mtrl-sci↗

arXiv2021

Decoherence of V$_{\rm B}^{-}$ spin defects in monoisotopic hexagonal boron nitride

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.

cond-mat.mtrl-sci↗

arXiv2021

Quantitative study of the response of a single NV defect in diamond to magnetic noise

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.

cond-mat.mes-hall↗

arXiv2020

Single photon wavefront-splitting interference: An illustration of the light quantum in action

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.

quant-ph↗

arXiv2020

Diamond spin sensors: A new way to probe nanomagnetism

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.

cond-mat.mtrl-sci↗

arXiv2020

Real-space imaging of non-collinear antiferromagnetic order with a single spin magnetometer

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.

cond-mat.mtrl-sci↗

arXiv2020

Effect of inter-system crossing rates and optical illumination on the polarization of nuclear spins nearby nitrogen-vacancy centers

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.

quant-ph↗

arXiv2020

Characterization of room-temperature in-plane magnetization in thin flakes of CrTe$_2$ with a single spin magnetometer

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.

cond-mat.mtrl-sci↗