The Charge Density Wave (CDW) state is a perfect example of a combined structural and electronic state, both characterized by a periodic lattice distortion and an electronic modulation of condensed electrons, resulting from electron-phonon coupling. They are thus prone to be tuned by lattice strain. NbSe3 is a prototypical example of CDW states, with a chain-like structure displaying two CDWs at 145K and 59K, with wavevectors along and inclined with respect to the chain axis b. Here, we report on the evolution of the lattice structure and CDW properties in the quasi-one-dimensional charge-density-wave system NbSe3 under tensile stresses applied along and perpendicular to the chains axis b by a combination of X-ray diffraction and transport measurements. We find that the lattice structure show exotic Poissons coefficients and strongly anisotropic Youngs moduli while the evolution of the electrical resistance demonstrates shifts of both charge-density-wave critical temperatures that are strongly correlated with the lattice parameters. The two CDW transitions display different behaviours under applied stresses, and suggest that a modification of the band curvature leads to the observed transport signatures.
Lattice deformation is a powerful way to engineer the properties of 2D materials, making their precise measurement an important challenge for both fundamental science and technological applications. Here, we demonstrate that boron-vacancy () 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 Raman mode in a multilayer hBN flake under uniaxial stress, establishing 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 centers, which will be valuable for future studies of strain-engineered 2D materials.
Magnetoelectric multiferroics are foreseen as paramount materials to control magnetism with an electric-field, targeting energy-efficient spintronics. The archetypal room-temperature antiferromagnetic ferroelectric, BiFeO3, harbors an incommensurate antiferromagnetic cycloid whose propagation direction is locked to ferroelectric domains. Epitaxial strain was shown to affect this antiferromagnetic ordering, stabilizing different cycloidal propagation directions, or a collinear antiferromagnetic state. Here we demonstrate the reversible, nonvolatile, electric-field triggered magnetic phase transition between two distinct antiferromagnetic states at room temperature. Using SrTiO3 vicinal substrates, we stabilize a single ferroelectric domain associated with a single antiferromagnetic cycloidal state in BiFeO3 epitaxial thin films. Electrically reversing the ferroelectric polarization deterministically within the same ferroelastic domain induces a reversible transition from a cycloidal to a collinear antiferromagnetic state, as directly visualized by scanning nitrogen vacancy (NV) magnetometry. These results bring insights into magnetoelectric devices for ultrafast and low-power spintronics.
Spin-defect-based quantum microscopy has recently made transformative advances in cutting-edge scientific research and technological innovation. The high sensitivity, high spatial resolution and excellent measurement modalities of quantum spin defects open up a range of opportunities at the forefront of condensed-matter physics research. Many of the advantages of this approach result from the quantum mechanical nature of the sensors, which offer functionalities that are not available with their classical counterparts. In this Review, we provide an overview of progress on scanning-probe nitrogen-vacancy quantum sensing research and its application to investigating the physics of emergent quantum materials with nanoscale spatial resolution. We also discuss quantum sensing platforms built on more recently discovered spin defects in one-dimensional and two-dimensional materials beyond nitrogen-vacancy centres. We conclude with an outlook on future directions and opportunities for these rapidly advancing quantum sensing technologies.
Color centers in silicon are emerging as promising platforms for quantum technologies. Among them, the G center has attracted considerable interest owing to its bright telecom O-band single-photon emission and its optically addressable metastable electron-spin triplet state. Here we investigate the spin properties of ensembles of G centers under above-band-gap excitation. We elucidate the spin photo-dynamics giving rise to the optical detected magnetic resonance (ODMR) response of G centers. The optimal pulsed sequence for measuring the ODMR spectrum of the G defects is identified, along with the temperature and optical-power regimes maximizing the spin readout contrast. Through magneto-optical measurements, we detect a level-anticrossing of the G center electron spin states. At last, we demonstrate coherent spin control of the defects, and characterize their spin-coherence properties. Unveiling the spin degree of freedom of the G center opens new avenues for the realization of quantum memories and quantum registers based on silicon color centers.
We demonstrate single-spin spectroscopy of a fluorescent tumbling defect in silicon called the "G center," behaving as a pseudomolecule randomly reorienting itself in the crystalline matrix. Using high-resolution spin spectroscopy, we reveal a fine magnetic structure resulting from the spin principal axes jumping between discrete orientations in the crystal. Modeling the atomic reorientation of the defect shows that spin tumbling induces variations in the coupling to the microwave magnetic field, enabling position-dependent Rabi frequencies to be detected in coherent spin control experiments. By virtue of its pseudomolecule configuration, the G center in silicon is a unique quantum system to investigate the mutual interaction between optical, spin, and rotation properties in a highly versatile material.
We perform sensitive nuclear magnetic resonance (NMR) with spin ensembles that are polarized by nitrogen-vacancy (NV) centers in diamond at room temperature. Using stabilized lasers, a balanced detection, and a highly uniform magnetic field, we resolve sharp NMR features arising from multiple spin clusters. In particular, we investigate the coupling between nuclear spins and NV centers in the neutral and negatively charged states. Further, we perform high-precision NMR and coherent control of families of C-13 nuclear spin ensembles in the vertical bar m(s) = 0) level of the NV ground state. Applying an off-axis magnetic field reveals the various sites associated with the otherwise degenerate couplings of the C-13 sites around the NV electronic spin, providing access to all the hyperfine tensor components. Finally, we observe spectroscopic signatures of pairs of nuclear spins coupled to the same NV center. These results are relevant for ensemble measurements of dynamical polarization that currently rely on expensive nuclear magnetic resonance systems as well as for recently proposed nuclear spin gyroscopes.
Lamellar crystalline materials, whose layers are bond by van der Waals forces, can be stacked to form ultrathin artificial heterostructures, and in particular vertical magnetic junctions when some of the stacked materials are (ferro)magnetic. Here, using the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$, we report a method for patterning lateral magnetic junctions. Exploiting the heat-induced phase transformation of the material into Cr$_x$Te$_y$ compounds ($x/y>1/2$), we use local laser heating to imprint patterns at the micron-scale. Optimizing laser heat dissipation, we further demonstrate the crucial role of the substrate to control the phase transformation. If plain, unstructured poorly heat-conducting substrates allow for direct writing of magnetic patterns, structured $h$-BN layers can serve as heat stencils to draw potentially thinner patterns. Besides, $h$-BN encapsulation turns out to be heat-protective (in addition from protecting against oxidation as it is generally used for), allowing the demonstration of room temperature ferromagnetism in $<$7~nm-thick 1$T$-CrTe$_2$.
Lamellar crystalline materials, whose layers are bound by van der Waals forces, can be stacked to form ultrathin artificial heterostructures and, in particular, vertical magnetic junctions when some of the stacked materials are (ferro)magnetic. Here, using the room temperature van der Waals ferromagnet 1T-CrTe2, we report a method for patterning lateral magnetic junctions. Exploiting the heat-induced phase transformation of the material into CrxTey compounds (x/y>1/2), we use local laser heating to imprint patterns at the micron-scale. Optimizing laser heat dissipation, we further demonstrate the crucial role of the substrate to control the phase transformation. If plain, unstructured poorly heat-conducting substrates allow for direct writing of magnetic patterns, structured h-BN layers can serve as heat stencils to draw potentially thinner patterns. Besides, h-BN encapsulation turns out to be heat-protective (in addition to protecting against oxidation, for which it is generally used), allowing the demonstration of room temperature ferromagnetism in <7 nm-thick 1T-CrTe2.
Les défauts ponctuels dans les solides sont des systèmes très prometteurs pour le développement de capteurs quantiques, dont les performances sont susceptibles de dépasser celles de leurs homologues classiques grâce à l’extrême sensibilité des systèmes quantiques élémentaires à leur environnement. Au sein de cette nouvelle famille de capteurs, le centre coloré NV du diamant est devenu une plateforme incontournable en raison de ses performances sans équivalent et de sa grande diversité d’applications, notamment pour l’imagerie magnétique à l’échelle nanométrique. Cet article décrit le principe de fonctionnement et les récents développements des capteurs et imageurs quantiques basés sur le centre NV du diamant.
We investigate the effect of confinement on the magnetic state of a 12 nm-thick Fe_5GeTe_2 layer grown by molecular beam epitaxy. We use quantitative scanning NV magnetometry to locally extract the magnetization in rectangular uniformly in-plane magnetized microstructures, showing no enhancement of the Curie temperature compared to magnetization measurements performed before patterning the film, in contrast to previous results obtained on thick Fe_3GeTe_2 flakes. Under the application of a weak out-of-plane magnetic field, we observe the stabilization of magnetic vortices at room temperature in micrometric squares. Finally, we highlight the effect of the size of the patterned micro-discs and micro-squares on the stabilization of the vortices using experiments and micromagnetic simulations. Our work thus proposes and demonstrates a way to stabilize non-collinear textures at room temperature in a van der Waals magnets using confinement, although we also show that this approach alone is not successful to enhance the Curie temperature of Fe_5GeTe_2 significantly above 300 K.
Boron vacancies (V_B^-) in hexagonal boron nitride (hBN) have emerged as a promising platform for two-dimensional quantum sensors capable of operating at atomic-scale proximity. However, the mechanisms responsible for photoluminescence quenching in thin hBN sensing layers when placed in contact with absorptive materials remain largely unexplored. In this Letter, we investigate non-radiative Förster resonance energy transfer (FRET) between V_B^- centers and either monolayer graphene or 2D semiconductors. Strikingly, we find that the FRET rate is negligible for hBN sensing layers thicker than 3 nm, highlighting the potential of V_B^- centers for integration into ultra-thin quantum sensors within van der Waals heterostructures. Furthermore, we experimentally extract the intrinsic radiative decay rate of V_B^- defects.
Electron spin resonance spectroscopy is a widely used technique for analyzing the microscopic structure, local environment and reorientation of atomic and molecular systems. Conventional inductive detection methods typically require to probe more than a billion of electron spins such that single atom motion is hidden through ensemble averaging. While several single spin spectroscopy methods are currently available, they have been so far limited to static systems. Here we demonstrate single spin spectroscopy of a fluorescent tumbling defect in silicon called the G center, behaving as a pseudo-molecule randomly reorienting itself in the crystalline matrix. Using high-resolution spin spectroscopy, we reveal a fine magnetic structure resulting from the spin principal axes jumping between discrete orientations in the crystal. By modeling the atomic reorientation of the defect, we demonstrate that spin tumbling induces variations in the coupling to the microwave magnetic field, enabling position-dependent Rabi frequencies to be detected in coherent spin control experiments. By virtue of its pseudo-molecule configuration, the G center in silicon is a unique quantum system to investigate the mutual interaction between optical, spin and rotation properties in a highly versatile material.
Magnon spintronics aims to harness spin waves in magnetic films for information technologies. Color center magnetometry is a promising tool for imaging spin waves, using electronic spins associated with atomic defects in solid-state materials as sensors. However, two main limitations persist: the magnetic fields required for spin-wave control detune the sensor-spin detection frequency, and this frequency is further restricted by the color center nature. Here, we overcome these limitations by decoupling the sensor spins from the spin-wave control fields -selecting color centers with intrinsic anisotropy axes orthogonal to the film magnetization- and by using color centers in diamond and hexagonal boron nitride to operate at complementary frequencies. We demonstrate isofrequency imaging of field-controlled spin waves in a magnetic half-plane and show how intrinsic magnetic anisotropies trigger bistable spin textures that govern spin-wave transport at device edges. Our results establish color center magnetometry as a versatile tool for advancing spin-wave technologies.
Charge transport in materials has an impact on a wide range of devices based on semiconductor, battery, or superconductor technology. Charge transport in sliding charge density waves (CDW) differs from all others in that the atomic lattice is directly involved in the transport process. To obtain an overall picture of the structural changes associated to the collective transport, the large coherent x-ray beam generated by an x-ray free-electron laser (XFEL) source was used. The CDW phase can be retrieved over the entire sample from diffracted intensities using a genetic algorithm. For currents below threshold, increasing shear deformation is observed in the central part of the sample while longitudinal deformation appears above threshold when shear relaxes. Shear thus precedes longitudinal deformation, with relaxation of one leading to the appearance of the other. Moreover, strain accumulates on surface steps in the sliding regime, demonstrating the strong pinning character of these surface discontinuities. The sliding process of nanometric CDW involves macroscopic sample dimensions.
Boron vacancies in hexagonal boron nitride (hBN) are among the most extensively studied optically active spin defects in van der Waals crystals, due to their promising potential to develop two-dimensional (2D) quantum sensors. In this letter, we demonstrate the tunability of the charge state of boron vacancies in ultrathin hBN layers, revealing a transition from the optically active singly negatively charged state to the optically inactive doubly negatively charged state when sandwiched between graphene electrodes. Notably, there is a photoluminescence quenching of a few percent upon the application of a bias voltage between the electrodes. Our findings emphasize the critical importance of considering the charge state of optically active defects in 2D materials, while also showing that the negatively charged boron vacancy remains robust against external perpendicular electric fields. This stability makes it a promising candidate for integration into various van der Waals heterostructures.
Among the wide variety of single fluorescent defects investigated in silicon, numerous studies have focused on color centers with a zero-phonon line around $1.28 \mu$m and identified to a common carbon-complex in silicon, namely the G center. However, inconsistent estimates regarding their quantum efficiency cast doubt on the correct identification of these individual emitters. Through a comparative analysis of their single-photon emission properties, we demonstrate that these single color centers are split in two distinct families of point defects. A first family consists of the genuine single G centers with a well-identified microscopic structure and whose photoluminescence has been investigated on ensemble measurements since the 60's. The remaining defects belong to a new color center, which we will refer to as G$^{\star}$ center, whose atomic configuration has yet to be determined. These results provide a safeguard against future defect misidentifications, which is crucial for further development of quantum technologies relying on G or G$^{\star}$ center quantum properties.
Topologically protected spin whirls in ferromagnets are foreseen as the cart-horse of solitonic information technologies. Nevertheless, the future of skyrmionics may rely on antiferromagnets due to their immunity to dipolar fields, straight motion along the driving force and ultrafast dynamics. While complex topological objects were recently discovered in intrinsic antiferromagnets, mastering their nucleation, stabilization and manipulation with energy-efficient means remains an outstanding challenge. Designing topological polar states in magnetoelectric antiferromagnetic multiferroics would allow one to electrically write, detect and erase topological antiferromagnetic entities. Here we stabilize ferroelectric centre states using a radial electric field in multiferroic BiFeO3 thin films. We show that such polar textures contain flux closures of antiferromagnetic spin cycloids, with distinct antiferromagnetic entities at their cores depending on the electric field polarity. By tuning the epitaxial strain, quadrants of canted antiferromagnetic domains can also be electrically designed. These results open the path to reconfigurable topological states in multiferroic antiferromagnets. Control over topological antiferromagnetic entities is achieved at room temperature in multiferroic nanodevices using an electric field that induces magnetoelectric coupling to ferroelectric centre states.
Among a broad diversity of color centers hosted in layered van der Waals materials, the negatively charged boron vacancy (VB-) center in hexagonal boron nitride (hBN) is garnering considerable attention for the development of quantum sensing units on a two-dimensional platform. In this work, we investigate how the optical response of an ensemble of VB- centers evolves with the hBN thickness in a range of a few to hundreds of nanometers. We show that the photoluminescence intensity features a nontrivial evolution with thickness, which is quantitatively reproduced by numerical calculations taking into account thickness-dependent variations of the absorption, radiative lifetime, and radiation pattern of VB- centers. Besides providing an important resource to optimize the performances of quantum sensing units based on VB- centers in hBN, the thickness-dependent nanophotonic effects discussed in this work generally apply to any type of color center embedded in a van der Waals material.
Magnetic skyrmions are topological magnetic textures that hold great promise as nanoscale bits of information in memory and logic devices. Although room-temperature ferromagnetic skyrmions and their current-induced manipulation have been demonstrated, their velocity has been limited to about 100 meters per second. In addition, their dynamics are perturbed by the skyrmion Hall effect, a motion transverse to the current direction caused by the skyrmion topological charge. Here, we show that skyrmions in compensated synthetic antiferromagnets can be moved by current along the current direction at velocities of up to 900 meters per second. This can be explained by the cancellation of the net topological charge leading to a vanishing skyrmion Hall effect. Our results open an important path toward the realization of logic and memory devices based on the fast manipulation of skyrmions in tracks.