Electron spin resonance (ESR) spectroscopy has broad applications in physics, chemistry and biology. As a complementary tool, zero-field ESR (ZF-ESR) spectroscopy has been proposed for decades and shown its own benefits for investigating the electron fine and hyperfine interaction. However, the ZF-ESR method has been rarely used due to the low sensitivity and the requirement of much larger samples than conventional ESR. In this work, we present a method for deploying ZF-ESR spectroscopy at the nanoscale by using a highly sensitive quantum sensor, the nitrogen-vacancy center in diamond. We also measure the nanoscale ZF-ESR spectrum of a few P1 centers in diamond, and show that the hyperfine coupling constant can be directly extracted from the spectrum. This method opens the door to practical applications of ZF-ESR spectroscopy, such as investigation of the structure and polarity information in spin-modified organic and biological systems.
Two-dimensional Nuclear Magnetic Resonance (NMR) is essential in molecular structure determination. The Nitrogen-Vacancy (NV) center in diamond has been proposed and developed as an outstanding quantum sensor to realize NMR in nanoscale. In this work, we develop a scheme for two-dimensional nanoscale NMR spectroscopy based on quantum controls on an NV center. We carry out a proof of principle experiment on a target of two coupled $^{13}$C nuclear spins in diamond. A COSY-like sequences is used to acquire the data on time domain, which is then converted to frequency domain with the fast Fourier…
Diamond quantum technologies based on color centers have rapidly emerged in the most recent years. The nitrogen-vacancy (NV) color center has attracted a particular interest, thanks to its outstanding spin properties and optical addressability. The NV center has been used to realize innovative multimode quantum-enhanced sensors that offer an unprecedented combination of high sensitivity and spatial resolution at room temperature. The technological progress and the widening of potential sensing applications have induced an increasing demand for performance advances of NV quantum sensors. Quantu…
Electron Spin Resonance (ESR) describes a suite of techniques for characterising electronic systems, with applications in physics, materials science, chemistry, and biology. However, the requirement for large electron spin ensembles in conventional ESR techniques limits their spatial resolution. Here we present a method for measuring the ESR spectrum of nanoscale electronic environments by measuring the relaxation time ($T_1$) of an optically addressed single-spin probe as it is systematically tuned into resonance with the target electronic system. As a proof of concept we extract the spectral…
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…
Quantum sensing exploits fundamental features of quantum mechanics and quantum control to realise sensing devices with potential applications in a broad range of scientific fields ranging from basic science to applied technology. The ultimate goal are devices that combine unprecedented sensitivity with excellent spatial resolution. Here, we propose a new platform for all-electric nanoscale quantum sensing based on a carbon nanotube double quantum dot. Our analysis demonstrates that the platform can achieve sensitivities that allow for the implementation of single-molecule magnetic resonance sp…
Precise timekeeping is critical to metrology, forming the basis by which standards of time, length and fundamental constants are determined. Stable clocks are particularly valuable in spectroscopy as they define the ultimate frequency precision that can be reached. In quantum metrology, where the phase of a qubit is used to detect external fields, the clock stability is defined by the qubit coherence time, which determines the spectral linewidth and frequency precision. Here we demonstrate a quantum sensing protocol where the spectral precision goes beyond the sensor coherence time and is limi…
We demonstrate a wide-band all-optical method of nanoscale magnetic resonance (MR) spectroscopy under ambient conditions. Our method relies on cross-relaxation between a probe spin, the electronic spin of a nitrogen-vacancy centre in diamond, and target spins as the two systems are tuned into resonance. By optically monitoring the spin relaxation time ($T_1$) of the probe spin while varying the amplitude of an applied static magnetic field, a frequency spectrum of the target spin resonances, a $T_1$-MR spectrum, is obtained. As a proof of concept, we measure $T_1$-MR spectra of a small ensembl…
Nuclear magnetic resonance (NMR) spectroscopy has approached the limit of single molecule sensitivity, however the spectral resolution is currently insufficient to obtain detailed information on chemical structure and molecular interactions. Here we demonstrate more than two orders of magnitude improvement in spectral resolution by performing correlation spectroscopy with shallow nitrogen-vacancy (NV) magnetic sensors in diamond. In principle, the resolution is sufficient to observe chemical shifts in $\sim$1 T magnetic fields, and is currently limited by molecular diffusion at the surface. We…
Observation of the Fano line shapes is essential to understand properties of the Fano resonance in different physical systems. We explore a tunable Fano resonance by tuning the phase shift in a Mach-Zehnder interferometer (MZI) based on a single-mode nano-optomechanical cavity. The Fano resonance is resulted from the optomechanically induced transparency caused by a nano-mechanical resonator and can be tuned by applying an optomechanical MZI. By tuning the phase shift in one arm of the MZI, we can observe the periodically varying line shapes of the Fano resonance, which represents an elaborate…
Classical sensors for spectrum analysis are widely used but lack micro- or nanoscale spatial resolution. On the other hand, quantum sensors, capable of working with nanoscale precision, do not provide precise frequency resolution over a wide range of frequencies. Using a single spin in diamond, we present a measurement protocol for quantum probes which enables full signal reconstruction on a nanoscale spatial resolution up to potentially 100\,GHz. We achieve $58\,\mathrm{nT/\sqrt{Hz}}$ amplitude and $0.095\,\mathrm{rad/\sqrt{Hz}}$ phase sensitivity and a relative frequency uncertainty of $10^{…
We report the nanoscale spin detection and electron paramagnetic resonance (EPR) spectrum of copper (Cu$^{2+}$) ions via double electron-electron resonance with single spins in diamond at room temperature and low magnetic fields. We measure unexpectedly narrow EPR resonances with linewidths $\sim 2-3$ MHz from copper-chloride molecules dissolved in poly-lysine. We also observe coherent Rabi oscillations and hyperfine splitting from single Cu$^{2+}$ ions, which could be used for dynamic nuclear spin polarization and higher sensitivity of spin detection. We interpret and analyze these observatio…
Nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) spectroscopy of bulk quantum materials have provided insight into phenomena such as quantum phase criticality, magnetism, and superconductivity. With the emergence of nanoscale 2-D materials with magnetic phenomena, inductively-detected NMR and NQR spectroscopy are not sensitive enough to detect the smaller number of spins in nanomaterials. The nitrogen-vacancy (NV) center in diamond has shown promise in bringing the analytic power of NMR and NQR spectroscopy to the nanoscale. However, due to depth-dependent formation effi…
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…
In nanoscale metrology applications, measurements are commonly limited by the performance of the sensor. Here we show that in nuclear magnetic resonance (NMR) spectroscopy measurements using single nitrogen-vacancy (NV) centers in diamond, the NV sensor electron spin limits spectral resolution down to a few hundred Hz, which constraints the characterization and coherent control of finite spin systems, and furthermore, is insufficient for high resolution NMR spectroscopy aiming at single molecule recognition and structure analysis of the latter. To overcome the limitation, we support an NV elec…
Nanoscale nuclear magnetic resonance (NMR) signals can be measured through hyperfine interaction to paramagnetic electron sensor spins. A heterodyne approach is widely used to overcome the electron spin lifetime limit in spectral resolution. It uses a series of modified Hahn echo pulse sequences applied coherently with precession signal resulting in a subsampled NMR signal. Due to challenges with applying high electron Rabi frequencies its application is limited to low fields, thus the full potential of the method is not yet exploited at high magnetic fields, beneficial for NMR. Here we presen…
Quantum Noise Spectroscopy of Nanoscale Charge Defects in Silicon Carbide at Room Temperature
School of Biomedical Engineering, Division of Life Sciences and Medicine, University of Science and Technology of China（中国科学技术大学生命科学与医学部生物医学工程学院）；Laboratory of Spin Magnetic Resonance, School of Physical Sciences, Anhui Province Key Laboratory of Scientific Instrument Development and Application, University of Science and Technology of China（中国科学技术大学物理学院自旋磁共振实验室、安徽省科学仪器开发与应用重点实验室）；Suzhou Institute for Advanced Research, University of Science and Technology of China（中国科学技术大学苏州高等研究院）；Hefei National Laboratory, University of Science and Technology of China（中国科学技术大学合肥国家实验室）
Magnetic resonance imaging (MRI) is a non-invasive and label-free technique widely used in medical diagnosis and life science research, and its success has benefited greatly from continuing efforts on enhancing contrast and resolution. Here we reported nanoscale MRI in a single cell using an atomic-size quantum sensor. With nitrogen-vacancy center in diamond, the intracellular protein ferritin has been imaged with a spatial resolution of ~ 10 nanometers, and ferritin-containing organelles were co-localized by correlative MRI and electron microscopy. Comparing to the current micrometer resoluti…
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…
Conventional nuclear magnetic resonance (NMR) spectroscopy relies on acquiring signal from a macroscopic ensemble of molecules to gain information about molecular structure and dynamics. Transferring this technique to nanoscale sample sizes would enable molecular analysis without the effects of averaging over spatial and temporal inhomogeneities and without the need for macroscopic volumes of analyte, both inherent to large ensemble measurements. Nanoscale NMR based on nitrogen vacancy (NV) centers inside bulk diamond chips achieves single nuclear spin sensitivity and the resolution required t…
Small solid state qubits, most prominently single spins in solids, can be remarkable sensors for various physical quantities ranging from magnetic fields to temperature. They package the performance of their bulk semiconductor counterparts into a nanoscale device, sometimes as small as a single atom. This review is a minimalist introduction into this concept. It gives a brief summary of quantum coherence, Ramsey spectroscopy and a derivation of the "standard quantum limit" of the sensitivity that a single-qubit sensor can reach. It goes on to discuss the surprising improvement that dynamical d…
We propose a scanning magnetic microscope which has a photoluminescence nanoprobe implanted in the tip of an AFM or STM, or NSOM, and exhibits optically detected magnetic resonance (ODMR). The proposed spin microscope has nanoscale lateral resolution and the single spin sensitivity for AFM and STM.
We investigate the potential for optical quantum technologies of Pr3+:Y2O3 in the form of monodisperse spherical nanoparticles. We measured optical inhomogeneous lines of 27 GHz, and optical homogeneous linewidths of 108 kHz and 315 kHz in particles of 400 nm and 150 nm average diameters respectively for the 1D2(0)--> 3H4(0) transition at 1.4 K. Furthermore, ground state and 1D2 excited state hyperfine structures in Y2O3 are here for the first time determined by spectral hole burning and modeled by complete Hamiltonian calculations. Ground-state spin transitions have energies of 5.99 MHz and 1…
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…
We revisit the phenomenon of quantum stochastic resonance in the regime of validity of the Bloch equations. We find that a stochastic resonance behavior in the steady-state response of the system is present whenever the noise-induced relaxation dynamics can be characterized via a single relaxation time scale. The picture is validated by a simple nuclear magnetic resonance experiment in water.
Gravitational resonance spectroscopy consists in measuring the energy spectrum of bouncing ultracold neutrons above a mirror by inducing resonant transitions between different discrete quantum levels. We discuss how to induce the resonances with a flow through arrangement in the GRANIT spectrometer, excited by an oscillating magnetic field gradient. The spectroscopy could be realized in two distinct modes (so called DC and AC) using the same device to produce the magnetic excitation. We present calculations demonstrating the feasibility of the newly proposed AC mode.
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…
Optical measurements of a nanoscale silicon optomechanical crystal cavity with a mechanical resonance frequency of 3.6GHz are performed at sub-kelvin temperatures. We infer optical-absorption-induced heating and damping of the mechanical resonator from measurements of phonon occupancy and motional sideband asymmetry. At the lowest probe power and lowest fridge temperature (10mK), the localized mechanical resonance is found to couple at a rate of 400Hz (Q=9x10^6) to a thermal bath of temperature 270mK. These measurements indicate that silicon optomechanical crystals cooled to millikelvin temper…
Water is the most important solvent in nature. It is a crucial issue to study interactions among water molecules. Nuclear magnetic resonance (NMR) spectroscopy is one of the most powerful tools to detect magnetic interactions for the structure analysis of a molecule with broad applications. But conventional NMR spectroscopy requires macroscopic sample quantities with hampers in investigating nanoscale structures. Through quantum control of a single spin quantum sensor, magnetic resonance spectroscopy of nanoscale organic molecules and single molecules has been achieved. However, the measuremen…
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 …
Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal…
Nitrogen-vacancy (NV) centers in diamond can be used for nanoscale sensing with atomic resolution and sensitivity; however, it has been observed that their properties degrade as they approach the diamond surface. Here we report that in addition to degraded spin coherence, NV centers within nanometers of the surface can also exhibit decreased fluorescence contrast for optically detected electron spin resonance (OD-ESR). We demonstrate that this decreased OD-ESR contrast arises from charge state dynamics of the NV center, and that it is strongly surface-dependent, indicating that surface enginee…
Nitrogen vacancy (NV) color centers in diamond are a leading modality for both superresolution optical imaging and nanoscale magnetic field sensing. In this work, we solve the remaining key challenge of performing optical magnetic imaging and spectroscopy selectively on multiple NV centers that are located within a diffraction-limited field-of-view. We use spin-RESOLFT microscopy to enable precision nanoscale mapping of magnetic field patterns with resolution down to ~20 nm, while employing a low power optical depletion beam. Moreover, we use a shallow NV to demonstrate the detection of proton…
The NV center in a diamond is a quantum sensor with exceptional quality for highly sensitive nanoscale analysis of NMR spectra and thermometry. In this study, we investigate nanoscale phase change detection of lipid bilayers utilizing ensemble-averaged nuclear spin detection from small volume ~ (6 nm)$^{3}$, which was determined by the depth of the NV center. Analysis of nanoscale NMR signal confirm thickness of lipid bilayer to be 6.2 nm $\pm$ 3.4 nm with proton density of 65 proton/nm$^{3}$ verifying formation of lipid bilayer on top of diamond sample. Correlation spectroscopy from nanoscale…
The statistical character of electron beams used in current technologies, as described by a stream of particles, is random in nature. Using coincidence measurements of femtosecond pulsed electron pairs, we report the observation of sub-Poissonian electron statistics that are non-random due to two-electron Coulomb interactions, and that exhibit an anti-bunching signal of 1 part in 4. This advancement is a fundamental step towards realizing a strongly quantum degenerate electron beam needed for many applications, and in particular electron correlation spectroscopy.
Feshbach resonances are among the essential control tools used in ultracold atom experiments. However, for complex atomic species the theoretical characterization of resonances becomes challenging. For closely spaced resonances, the measurement of three-body losses does not provide sufficient resolution to discriminate them. For this reason, resonance spectroscopy of trapped isolated atoms is becoming the state of the art. Here we show that trapping the atoms in a double well potential such as an optical lattice or a pair of optical tweezers enables precise characterization of not only the res…
A realization of the force-induced remnant magnetization spectroscopy (FIRMS) technique of specific biomolecular binding is presented where detection is accomplished with wide-field optical and diamond-based magnetometry using an ensemble of nitrogen-vacancy (NV) color centers. The technique may be adapted for massively parallel screening of arrays of nanoscale samples.
