The ability to perform nanoscale electric field imaging of elementary charges at ambient temperatures will have diverse interdisciplinary applications. While the nitrogen-vacancy (NV) center in diamond is capable of high-sensitivity electrometry, demonstrations have so far been limited to macroscopic field features or detection of single charges internal to diamond itself. In this work we greatly extend these capabilities by using a shallow NV center to image the electric field of a charged atomic force microscope tip with nanoscale resolution. This is achieved by measuring Stark shifts in the NV spin-resonance due to AC electric fields. To achieve this feat we employ for the first time, the integration of Qdyne with scanning quantum microscopy. We demonstrate near single charge sensitivity of $η_e = 5.3$ charges/$\sqrt{\text{Hz}}$, and sub-charge detection ($0.68e$). This proof-of-concept experiment provides the motivation for further sensing and imaging of electric fields using NV centers in diamond.
Solid-state quantum emitters, such as artificially engineered quantum dots or naturally occurring defects in solids, are being investigated for applications ranging from quantum information science and optoelectronics to biomedical imaging. Recently, these same systems have also been studied from the perspective of nanoscale metrology. In this letter we study the near-field optical properties of a diamond nanocrystal hosting a single nitrogen vacancy center. We find that the nitrogen vacancy center is a sensitive probe of the surrounding electromagnetic mode structure. We exploit this sensitiv…
Nitrogen-vacancy (NV) centers in diamond can be used as quantum sensors to image the magnetic field with nanoscale resolution. However, nanoscale electric-field mapping has not been achieved so far because of the relatively weak coupling strength between NV and electric field. Using individual shallow NVs, here we succeeded to quantitatively image the contours of electric field from a sharp tip of a qPlus-based atomic force microscope (AFM), and achieved a spatial resolution of ~10 nm. Through such local electric fields, we demonstrated electric control of NV's charge state with sub-5 nm preci…
The electrical conductivity of a material can feature subtle, nontrivial, and spatially-varying signatures with critical insight into the material's underlying physics. Here we demonstrate a conductivity imaging technique based on the atom-sized nitrogen-vacancy (NV) defect in diamond that offers local, quantitative, and noninvasive conductivity imaging with nanoscale spatial resolution. We monitor the spin relaxation rate of a single NV center in a scanning probe geometry to quantitatively image the magnetic fluctuations produced by thermal electron motion in nanopatterned metallic conductors…
Optically-detected magnetic resonance using Nitrogen Vacancy (NV) color centres in diamond is a leading modality for nanoscale magnetic field imaging, as it provides single electron spin sensitivity, three-dimensional resolution better than 1 nm, and applicability to a wide range of physical and biological samples under ambient conditions. To date, however, NV-diamond magnetic imaging has been performed using real space techniques, which are either limited by optical diffraction to 250 nm resolution or require slow, point-by-point scanning for nanoscale resolution, e.g., using an atomic force …
This work demonstrates nanoscale magnetic imaging using bright circularly polarized high-harmonic radiation. We utilize the magneto-optical contrast of worm-like magnetic domains in a Co/Pd multilayer structure, obtaining quantitative amplitude and phase maps by lensless imaging. A diffraction-limited spatial resolution of 49 nm is achieved with iterative phase reconstruction enhanced by a holographic mask. Harnessing the unique coherence of high harmonics, this approach will facilitate quantitative, element-specific and spatially-resolved studies of ultrafast magnetization dynamics, advancing…
Topological states of light represent counterintuitive optical modes localized at boundaries of finite-size optical structures that originate from the properties of the bulk. Being defined by bulk properties, such boundary states are insensitive to certain types of perturbations, thus naturally enhancing robustness of photonic circuitries. Conventionally, the N-dimensional bulk modes correspond to (N-1)-dimensional boundary states. The higher-order bulk-boundary correspondence relates N-dimensional bulk to boundary states with dimensionality reduced by more than 1. A special interest lies in m…
We present a novel spectroscopy protocol based on optimal control of a single quantum system. It enables measurements with quantum-limited sensitivity (η_ω~ 1/sqrt(T_2^*),T_2^* denoting the system's coherence time) but has an orders of magnitude larger dynamic range than pulsed spectroscopy methods previously employed for this task. We employ this protocol to image nanoscale magnetic fields with a single scanning NV center in diamond. Here, our scheme enables quantitative imaging of a strongly inhomogeneous field in a single scan without closed-loop control, which has previously been necessary…
Controllable atomic-scale quantum systems hold great potential as sensitive tools for nanoscale imaging and metrology. Possible applications range from nanoscale electric and magnetic field sensing to single photon microscopy, quantum information processing, and bioimaging. At the heart of such schemes is the ability to scan and accurately position a robust sensor within a few nanometers of a sample of interest, while preserving the sensor's quantum coherence and readout fidelity. These combined requirements remain a challenge for all existing approaches that rely on direct grafting of individ…
We report a method for accelerated nanoscale nuclear magnetic resonance imaging by detecting several signals in parallel. Our technique relies on phase multiplexing, where the signals from different nuclear spin ensembles are encoded in the phase of an ultrasensitive magnetic detector. We demonstrate this technique by simultaneously acquiring statistically polarized spin signals from two different nuclear species (1H, 19F) and from up to six spatial locations in a nanowire test sample using a magnetic resonance force microscope. We obtain one-dimensional imaging resolution better than 5 nm, an…
The detection of ensembles of spins under ambient conditions has revolutionized the biological, chemical, and physical sciences through magnetic resonance imaging and nuclear magnetic resonance. Pushing sensing capabilities to the individual-spin level would enable unprecedented applications such as single molecule structural imaging; however, the weak magnetic fields from single spins are undetectable by conventional far-field resonance techniques. In recent years, there has been a considerable effort to develop nanoscale scanning magnetometers, which are able to measure fewer spins by bringi…
Second harmonic generation (SHG) is a nonlinear optical response arising exclusively from broken inversion symmetry in the electric-dipole limit. Recently, SHG has attracted widespread interest as a versatile and noninvasive tool for characterization of crystal symmetry and emerging ferroic or topological orders in quantum materials. However, conventional far-field optics is unable to probe local symmetry at the deep subwavelength scale. Here, we demonstrate near-field SHG imaging of 2D semiconductors and heterostructures with the spatial resolution down to 20 nm using a scattering-type nano-o…
The low-temperature electrical resistivity of corrugated semiconductor films is theoretically considered. Nanoscale corrugation enhances the electron-electron scattering contribution to the resistivity, resulting in a stepwise resistivity development with increasing corrugation amplitude. The enhanced electron scattering is attributed to the curvature-induced potential energy that affects the motion of electrons confined to a thin curved film. Geometric conditions and microscopic mechanism of the stepwise resistivity are discussed in detail.
Recent developments in x-ray science provide methods to probe deeply embedded mesoscale grain structures and spatially resolve them using dark field x-ray microscopy (DFXM). Extending this technique to investigate weak diffraction signals such as magnetic systems, quantum materials and thin films proves challenging due to available detection methods and incident x-ray flux at the sample. We present a direct detection method focusing on DFXM studies in the hard x-ray range of 10s of keV and above capable of approaching nanoscale resolution. Additionally, we compare this direct detection scheme …
We report a photoluminescence imaging system for locating single quantum emitters with respect to alignment features. Samples are interrogated in a 4~K closed-cycle cryostat by a high numerical aperture (NA=0.9, 100$\times$ magnification) objective that sits within the cryostat, enabling high efficiency collection of emitted photons without image distortions due to the cryostat windows. The locations of single InAs/GaAs quantum dots within a $>50$~$μ$m~$\times$~50~$μ$m field of view are determined with $\approx4.5$~nm uncertainty (one standard deviation) in a 1~s long acquisition. The uncertai…
We present an implementation of all-diamond scanning probes for scanning nitrogen-vacancy (NV) magnetometry fabricated from (111)-oriented diamond material. The realized scanning probe tips on average contain single NV spins, a quarter of which have their spin quantization axis aligned parallel to the tip direction. Such tips enable single-axis vector magnetic field imaging with nanoscale resolution, where the measurement axis is oriented normal to the scan plane. We discuss how these tips bring multiple practical advantages for NV magnetometry, in particular regarding quantitative analysis of…
Quantum control of individual spins in condensed matter systems is an emerging field with wide-ranging applications in spintronics, quantum computation, and sensitive magnetometry. Recent experiments have demonstrated the ability to address and manipulate single electron spins through either optical or electrical techniques. However, it is a challenge to extend individual spin control to nanoscale multi-electron systems, as individual spins are often irresolvable with existing methods. Here we demonstrate that coherent individual spin control can be achieved with few-nm resolution for proximal…
Nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are well-established techniques that provide valuable information in a diverse set of disciplines but are currently limited to macroscopic sample volumes. Here we demonstrate nanoscale NMR spectroscopy and imaging under ambient conditions of samples containing multiple nuclear species, using nitrogen-vacancy (NV) colour centres in diamond as sensors. With single, shallow NV centres in a diamond chip and samples placed on the diamond surface, we perform NMR spectroscopy and one-dimensional MRI on few-nanometre-sized samples c…
Nitrogen-vacancy (NV) center in diamond is a promising quantum sensor with remarkably versatile sensing capabilities. While scanning NV magnetometry is well-established, NV electrometry has been so far limited to bulk diamonds. Here we demonstrate imaging external alternating (AC) and direct (DC) electric fields with a single NV at the apex of a diamond scanning tip under ambient conditions. A strong electric field screening effect is observed at low frequencies due to charge noise on the surface. We quantitatively measure its frequency dependence, and overcome this screening by mechanically o…
We report on imaging of microwave (MW) magnetic fields using a magnetometer based on the electron spin of a nitrogen vacancy center in diamond. We quantitatively image the magnetic field generated by high frequency (GHz) MW current with nanoscale resolution using a scanning probe technique. We demonstrate a MW magnetic field sensitivity in the range of a few nT/$\sqrt{\text{Hz}}$, polarization selection and broadband capabilities under ambient conditions and thereby establish the nitrogen vacancy center a versatile and high performance tool for the detection of MW fields. As a first applicatio…
We investigate the electronic and structural changes at the nanoscale in vanadium dioxide (VO2) in the vicinity of its thermally driven phase transition. Both electronic and structural changes exhibit phase coexistence leading to percolation. In addition, we observe a dichotomy between the local electronic and structural transitions. Nanoscale x-ray diffraction reveals local, non-monotonic switching of the lattice structure, a phenomenon that is not seen in the electronic insulator-to-metal transition mapped by near-field infrared microscopy.
Magnetic microscopy that combines nanoscale spatial resolution with picosecond scale temporal resolution uniquely enables direct observation of the spatiotemporal magnetic phenomena that are relevant to future high-speed, high-density magnetic storage and logic technologies. Magnetic microscopes that combine these metrics has been limited to facility-level instruments. To address this gap in lab-accessible spatiotemporal imaging, we develop a time-resolved near-field magnetic microscope based on magneto-thermal interactions. We demonstrate both magnetization and current density imaging modalit…
Spin defects like the negatively charged boron vacancy color center ($V_B^-$) in hexagonal boron nitride (hBN) may enable new forms of quantum sensing with near-surface defects in layered van der Waals heterostructures. Here, we reveal the effect of strain associated with creases in hBN flakes on $V_B^-$ and $V_B$ color centers in hBN with correlative cathodoluminescence and photoluminescence microscopies. We observe strong localized enhancement and redshifting of the $V_B^-$ luminescence at creases, consistent with density functional theory calculations showing $V_B^-$ migration toward region…
We present a method for nanoscale thermal imaging of insulating thin films using atomic force microscopy (AFM), and we demonstrate its utility on VO$_2$. We sweep the applied voltage $V$ to a conducting AFM tip in contact mode and measure the local current $I$ through the film. By fitting the $IV$ curves to a Poole-Frenkel conduction model at low $V$, we calculate the local temperature with spatial resolution better than 50 nm using only fundamental constants and known film properties. Our thermometry technique enables local temperature measurement of \textit{any} insulating film dominated by …
Many promising building blocks of future electronic technology - including non-stoichiometric compounds, strongly correlated oxides, and strained or patterned films - are inhomogeneous on the nanometer length scale. Exploiting the inhomogeneity of such materials to design next-generation nanodevices requires a band structure probe with nanoscale spatial resolution. To address this demand, we report the first simultaneous observation and quantitative reconciliation of two candidate probes - Landau level spectroscopy and quasiparticle interference imaging - which we employ here to reconstruct th…
Charge transport in nanostructures and thin films is fundamental to many phenomena and processes in science and technology, ranging from quantum effects and electronic correlations in mesoscopic physics, to integrated charge- or spin-based electronic circuits, to photoactive layers in energy research. Direct visualization of the charge flow in such structures is challenging due to their nanometer size and the itinerant nature of currents. In this work, we demonstrate non-invasive magnetic imaging of current density in two-dimensional conductor networks including metallic nanowires and carbon n…
This paper presents the design and fabrication of batch-processed cantilever probes with electrical shielding for scanning microwave impedance microscopy. The diameter of the tip apex, which defines the electrical resolution, is less than 50 nm. The width of the stripline and the thicknesses of the insulation dielectrics are optimized for a small series resistance (< 5 W) and a small background capacitance (~ 1 pF), both critical for high sensitivity imaging on various samples. The coaxial shielding ensures that only the probe tip interacts with the sample. The structure of the cantilever is d…
The nitrogen-vacancy (NV) center is a potential atomic-scale spin sensor for electric field sensing. However, its natural susceptibility to the magnetic field hinders effective detection of the electric field. Here we propose a robust electrometric method utilizing continuous dynamic decoupling (CDD) technique. During the CDD period, the NV center evolves in a dressed-state space, where the sensor is resistant to magnetic fields but remains sensitive to electric fields. As an example, we use this method to isolate the electric noise from a complex electro-magnetical environment near diamond su…
The Clausius inequality, one of the classical formulations of the second law, was recently found to be violated in the quantum regime. Here this result is formulated in the context of a mesoscopic or nanoscale linear RLC circuit interacting with a thermal bath. Previous experiments in this and related fields are analyzed and possibilities of experimental detection of the violation are pointed out. It is discussed that recent experiments reached the range of temperatures, where the effect should be visible, and that a part of the proposal was already confirmed.
We use apertureless scattering near-field optical microscopy (SNOM) to investigate the nanoscale optical response of vanadium dioxide (VO2) thin films through a temperature-induced insulator-to-metal transition (IMT). We compare images of the transition at both mid-infrared (MIR) and terahertz (THz) frequencies, using a custom-built broadband THz-SNOM compatible with both cryogenic and elevated temperatures. We observe that the character of spatial inhomogeneities in the VO2 film strongly depends on the probing frequency. In addition, we find that individual insulating (or metallic) domains ha…
Spin-labeling of molecules with paramagnetic ions is an important approach for determining molecular structure, however current ensemble techniques lack the sensitivity to detect few isolated spins. In this Letter, we demonstrate two-dimensional nanoscale imaging of paramagnetic gadolinium compounds using scanning relaxometry of a single nitrogen vacancy (NV) center in diamond. Gadopentetate dimeglumine attached to an atomic force microscope tip is controllably interacted with and detected by the NV center, by virtue of the fact that the NV exhibits fast relaxation in the fluctuating magnetic …
Time-domain Brillouin scattering is an all-optical experimental technique based on ultrafast lasers applied for generation and detection of coherent acoustic pulses on time durations of picoseconds and length scales of nanometers. In transparent materials scattering of the probe laser beam by the coherent phonons permits imaging of sample inhomogeneity. The transient optical reflectivity of the sample recorded by the probe beam as the acoustic nanopulse propagates in space contains information on the acoustical, optical, and acousto-optical parameters of the material under study. The experimen…
Nanoscale phase coexistence and inhomogeneity are ubiquitous in correlated electron materials, existing in doped Mott insulators, manganites, and high-temperature superconductors. The small length scales and lack of contrast mechanisms make it extremely challenging to measure real-space images of the phase coexistence with high resolution. Yet, images aid our understanding of how phase coexistence and domain boundaries dictate the exotic material properties. Here we show that resonant soft-X-ray holography, previously employed to image magnetic domains, can be used to image phase separation on…
We report the nanoscale conductivity imaging of correlated electronic states in angle-aligned WSe2/WS2 heterostructures using microwave impedance microscopy. The noncontact microwave probe allows us to observe the Mott insulating state with one hole per moiré unit cell that persists for temperatures up to 150 K, consistent with other characterization techniques. In addition, we identify for the first time a Mott insulating state at one electron per moiré unit cell. Appreciable inhomogeneity of the correlated states is directly visualized in the hetero-bilayer region, indicative of local disord…
Magnetic-domain structure and dynamics play an important role in understanding and controlling the magnetic properties of two-dimensional magnets, which are of interest to both fundamental studies and applications[1-5]. However, the probe methods based on the spin-dependent optical permeability[1,2,6] and electrical conductivity[7-10] can neither provide quantitative information of the magnetization nor achieve nanoscale spatial resolution. These capabilities are essential to image and understand the rich properties of magnetic domains. Here, we employ cryogenic scanning magnetometry using a s…
Individual, luminescent point defects in solids so called color centers are atomic-sized quantum systems enabling sensing and imaging with nanoscale spatial resolution. In this overview, we introduce nanoscale sensing based on individual nitrogen vacancy (NV) centers in diamond. We discuss two central challenges of the field: First, the creation of highly-coherent, shallow NV centers less than 10 nm below the surface of single-crystal diamond. Second, the fabrication of tip-like photonic nanostructures that enable efficient fluorescence collection and can be used for scanning probe imaging bas…
We describe a new type of scanning probe microscope based on a superconducting quantum interference device (SQUID) that resides on the apex of a sharp tip. The SQUID-on-tip is glued to a quartz tuning fork which allows scanning at a tip-sample separation of a few nm. The magnetic flux sensitivity of the SQUID is 1.8 μ_0/Hz^{1/2} and the spatial resolution is about 200 nm, which can be further improved. This combination of high sensitivity, spatial resolution, bandwidth, and the very close proximity to the sample provides a powerful tool for study of dynamic magnetic phenomena on the nanoscale.…
One-dimensional nanoscale devices, such as semiconductor nanowires (NWs) and single- walled carbon nanotubes (SWNTs), have been intensively investigated because of their potential application of future high-speed electronic, optoelectronic, and sensing devices. To overcome current limitations on the speed of contemporary devices, investigation of charge carrier dynamics with an ultrashort time scale is one of the primary steps necessary for developing high-speed devices. In the present study, we visualize ultrafast carrier dynamics in nanoscale devices using a combination of scanning photocurr…
Following the lifespan of optical excitations from their creation to decay into photons is crucial in understanding materials optical properties. Macroscopically, techniques such as the photoluminescence excitation spectroscopy provide unique information on the photophysics of materials with applications as diverse as quantum optics or photovoltaics. Materials excitation and emission pathways are affected by nanometer scale variations directly impacting devices performances. However, they cannot be directly accessed, despite techniques, such as optical spectroscopies with free electrons, havin…
In monolayer transition metal dichalcogenides, quantum emitters are associated with localized strain that can be deterministically applied to create designer nano-arrays of single photon sources. Despite an overwhelming empirical correlation with local strain, the nanoscale interplay between strain, excitons, defects and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopy of excitons in nanobubbles of localized strain in monolayer WSe2 with atomistic structural models to elucidate ho…
The nitrogen-vacancy (NV) centre in diamond is a leading platform for nanoscale sensing and imaging, as well as quantum information processing in the solid state. To date, individual control of two NV electronic spins at the nanoscale has been demonstrated. However, a key challenge is to scale up such control to arrays of NV spins. Here we apply nanoscale magnetic resonance frequency encoding to realize site-selective addressing and coherent control of a four-site array of NV spins. Sites in the array are separated by 100 nm, with each site containing multiple NVs separated by ~15 nm. Microcoi…
The ability to probe nanoscale heat flow in a material is often limited by lack of spatial resolution. Here, we use a diamond-nanocrystal-hosted nitrogen-vacancy centre attached to the apex of a silicon thermal tip as a local temperature sensor. We apply an electrical current to heat up the tip and rely on the NV to monitor the thermal changes the tip experiences as it is brought into contact with surfaces of varying thermal conductivity. With the aid of a combined AFM/confocal setup, we image phantom microstructures with nanoscale resolution, and attain excellent agreement between the thermal…
Planar scanning probe microscopy enables vector magnetic field imaging at the nanoscale
University of Rostock（罗斯托克大学）；Fraunhofer Institute for Applied Solid State Physics（弗劳恩霍夫应用固态物理研究所）；Walther-Meißner-Institut, Bayerische Akademie der Wissenschaften（瓦尔特-迈斯纳研究所，巴伐利亚科学院）；Technical University of Munich（慕尼黑工业大学）
We investigate a nanoscale dielectric capacitor model consisting of two-dimensional, hexagonal h-BN layers placed between two commensurate and metallic graphene layers using self-consistent field density functional theory. The separation of equal amounts of electric charge of different sign in different graphene layers is achieved by applying electric field perpendicular to the layers. The stored charge, energy, and the electric potential difference generated between the metallic layers are calculated from the first-principles for the relaxed structures. Predicted high-capacitance values exhib…
Spin waves modes in magnetic waveguides with width down to 320 nm have been studied by electrical propagating spin-wave spectroscopy and micromagnetic simulations for both longitudinal and transverse magnetic bias fields. For longitudinal bias fields, a 1.3 GHz wide spin-wave band was observed in agreement with analytical dispersion relations for uniform magnetization. However, transverse bias field led to several distinct bands, corresponding to different quantized width modes, with both negative and positive slopes. Micromagnetic simulations showed that, in this geometry, the magnetization w…
Microscopic studies of superconductors and their vortices play a pivotal role in our understanding of the mechanisms underlying superconductivity. Local measurements of penetration depths or magnetic stray-fields enable access to fundamental aspects of superconductors such as nanoscale variations of superfluid densities or the symmetry of their order parameter. However, experimental tools, which offer quantitative, nanoscale magnetometry and operate over the large range of temperature and magnetic fields relevant to address many outstanding questions in superconductivity, are still missing. He…
Methods for nanoscale material characterization are in ever-increasing demand, especially those that can provide a broader range of information at once. Near-field techniques based on combinations of scanning probe microscopy (SPM) and Raman or photoluminescence (PL) spectroscopy (tip-enhanced Raman spectroscopy [TERS] and/or tip-enhanced photoluminescence [TEPL]) are, thanks to their capabilities and fast development, strong candidates for becoming widespread across the scientific community as SPM and Raman microscopy did only a decade or two ago. Herein, a gap-less TEPL study is performed di…
Raman-detected quantum dot microscopy for nanoscale electrostatic potential imaging
Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences（捷克科学院有机化学与生物化学研究所）；Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）；Faculty of Mathematics and Physics, Charles University（查理大学数学与物理学院）
Many classes of two-dimensional (2D) materials have emerged as potential platforms for novel electronic and optical devices. However, the physical properties are strongly influenced by nanoscale heterogeneities in the form of edges, grain boundaries, and nucleation sites. Using combined tip-enhanced Raman scattering (TERS) and photoluminescence (TEPL) nano-spectroscopy and -imaging, we study the associated effects on the excitonic properties in monolayer WSe2 grown by physical vapor deposition (PVD). With <15 nm spatial resolution we resolve nonlocal nanoscale correlations of PL spectral inten…
Energy dissipation is a fundamental process governing the dynamics of physical, chemical, and biological systems. It is also one of the main characteristics distinguishing quantum and classical phenomena. In condensed matter physics, in particular, scattering mechanisms, loss of quantum information, or breakdown of topological protection are deeply rooted in the intricate details of how and where the dissipation occurs. Despite its vital importance the microscopic behavior of a system is usually not formulated in terms of dissipation because the latter is not a readily measureable quantity on …
Optical detection of nanoscale objects without relying on fluorescence is a current challenge due to their extremely weak interaction with light. Resonator-enhanced absorption microscopy is a novel tool to heavily boost the light-matter interaction. It combines highly sensitive, spatially resolved imaging with spectroscopy, offering a competitive alternative to established methods for the detection and analysis of nanoscale systems in nanotechnology, material design, and the life sciences.
