Nanoscale imaging magnetometry with diamond spins under ambient conditions

Magnetic resonance imaging and optical microscopy are key technologies in the life sciences. For microbiological studies, especially of the inner workings of single cells, optical microscopy is normally used because it easily achieves resolution close to the optical wavelength. But in conventional microscopy, diffraction limits the resolution to about half the wavelength. Recently, it was shown that this limit can be partly overcome by nonlinear imaging techniques, but there is still a barrier to reaching the molecular scale. In contrast, in magnetic resonance imaging the spatial resolution is not determined by diffraction; rather, it is limited by magnetic field sensitivity, and so can in principle go well below the optical wavelength. The sensitivity of magnetic resonance imaging has recently been improved enough to image single cells, and magnetic resonance force microscopy has succeeded in detecting single electrons and small nuclear spin ensembles. However, this technique currently requires cryogenic temperatures, which limit most potential biological applications. Alternatively, single-electron spin states can be detected optically, even at room temperature in some systems. Here we show how magneto-optical spin detection can be used to determine the location of a spin associated with a single nitrogen-vacancy centre in diamond with nanometre resolution under ambient conditions. By placing these nitrogen-vacancy spins in functionalized diamond nanocrystals, biologically specific magnetofluorescent spin markers can be produced. Significantly, we show that this nanometre-scale resolution can be achieved without any probes located closer than typical cell dimensions. Furthermore, we demonstrate the use of a single diamond spin as a scanning probe magnetometer to map nanoscale magnetic field variations. The potential impact of single-spin imaging at room temperature is far-reaching. It could lead to the capability to probe biologically relevant spins in living cells.     

Optimizing ultrasensitive single electron magnetometer based on nitrogen-vacancy center in diamond

The measurement of the weak magnetic field in nanoscale resolution and at room temperature is always a significant topic in biological, physical, and material science. Such detection can be used to decide the characterization of the samples, such as cells, materials, and so on. Nitrogen-vacancy (NV) center in diamond has been proved to be able to detect a magnetic field with nano Tesla sensitivity and nanometer resolution at room temperature. Here we experimentally demonstrate an optimized NV center based single electron magnetometer in a commercial diamond and under a home-built optically detected magnetic resonance (ODMR) microscope. With current technology, we change the optically detected time window to get a better signal to noise ratio, and use dynamical decoupling to increase the slope of magnetic field amplitude versus fluorescence signal. By employing the 8-pulse XY-4 dynamical decoupling sequence we achieve a sensitivity of 18.9 nT (Hz)(1/2) , which is 1.7 times better than spin echo. We also propose a NV center based scanning diamond microscope for electron and nuclear spins detection as well as nanoscale magnetic resonance imaging. If it is realized, the NV center based magnetometry will have wide application in the future.     

Single spin detection by magnetic resonance force microscopy

Magnetic resonance imaging (MRI) is well known as a powerful technique for visualizing subsurface structures with three-dimensional spatial resolution. Pushing the resolution below 1 micro m remains a major challenge, however, owing to the sensitivity limitations of conventional inductive detection techniques. Currently, the smallest volume elements in an image must contain at least 10(12) nuclear spins for MRI-based microscopy, or 10(7) electron spins for electron spin resonance microscopy. Magnetic resonance force microscopy (MRFM) was proposed as a means to improve detection sensitivity to the single-spin level, and thus enable three-dimensional imaging of macromolecules (for example, proteins) with atomic resolution. MRFM has also been proposed as a qubit readout device for spin-based quantum computers. Here we report the detection of an individual electron spin by MRFM. A spatial resolution of 25 nm in one dimension was obtained for an unpaired spin in silicon dioxide. The measured signal is consistent with a model in which the spin is aligned parallel or anti-parallel to the effective field, with a rotating-frame relaxation time of 760 ms. The long relaxation time suggests that the state of an individual spin can be monitored for extended periods of time, even while subjected to a complex set of manipulations that are part of the MRFM measurement protocol.     

Single-shot read-out of an individual electron spin in a quantum dot

Spin is a fundamental property of all elementary particles. Classically it can be viewed as a tiny magnetic moment, but a measurement of an electron spin along the direction of an external magnetic field can have only two outcomes: parallel or anti-parallel to the field. This discreteness reflects the quantum mechanical nature of spin. Ensembles of many spins have found diverse applications ranging from magnetic resonance imaging to magneto-electronic devices, while individual spins are considered as carriers for quantum information. Read-out of single spin states has been achieved using optical techniques, and is within reach of magnetic resonance force microscopy. However, electrical read-out of single spins has so far remained elusive. Here we demonstrate electrical single-shot measurement of the state of an individual electron spin in a semiconductor quantum dot. We use spin-to-charge conversion of a single electron confined in the dot, and detect the single-electron charge using a quantum point contact; the spin measurement visibility is approximately 65%. Furthermore, we observe very long single-spin energy relaxation times (up to approximately 0.85 ms at a magnetic field of 8 T), which are encouraging for the use of electron spins as carriers of quantum information.     

Electrical detection of the spin resonance of a single electron in a silicon field-effect transistor

The ability to manipulate and monitor a single-electron spin using electron spin resonance is a long-sought goal. Such control would be invaluable for nanoscopic spin electronics, quantum information processing using individual electron spin qubits and magnetic resonance imaging of single molecules. There have been several examples of magnetic resonance detection of a single-electron spin in solids. Spin resonance of a nitrogen-vacancy defect centre in diamond has been detected optically, and spin precession of a localized electron spin on a surface was detected using scanning tunnelling microscopy. Spins in semiconductors are particularly attractive for study because of their very long decoherence times. Here we demonstrate electrical sensing of the magnetic resonance spin-flips of a single electron paramagnetic spin centre, formed by a defect in the gate oxide of a standard silicon transistor. The spin orientation is converted to electric charge, which we measure as a change in the source/drain channel current. Our set-up may facilitate the direct study of the physics of spin decoherence, and has the practical advantage of being composed of test transistors in a conventional, commercial, silicon integrated circuit. It is well known from the rich literature of magnetic resonance studies that there sometimes exist structural paramagnetic defects near the Si/SiO2 interface. For a small transistor, there might be only one isolated trap state that is within a tunnelling distance of the channel, and that has a charging energy close to the Fermi level.     

Detecting excitation and magnetization of individual dopants in a semiconductor

An individual magnetic atom doped into a semiconductor is a promising building block for bottom-up spintronic devices and quantum logic gates. Moreover, it provides a perfect model system for the atomic-scale investigation of fundamental effects such as magnetism in dilute magnetic semiconductors. However, dopants in semiconductors so far have not been studied by magnetically sensitive techniques with atomic resolution that correlate the atomic structure with the dopant's magnetism. Here we show electrical excitation and read-out of a spin associated with a single magnetic dopant in a semiconductor host. We use spin-resolved scanning tunnelling spectroscopy to measure the spin excitations and the magnetization curve of individual iron surface-dopants embedded within a two-dimensional electron gas confined to an indium antimonide (110) surface. The dopants act like isolated quantum spins the states of which are governed by a substantial magnetic anisotropy that forces the spin to lie in the surface plane. This result is corroborated by our first principles calculations. The demonstrated methodology opens new routes for the investigation of sample systems that are more widely studied in the field of spintronics-that is, Mn in GaAs (ref. 5), magnetic ions in semiconductor quantum dots, nitrogen-vacancy centres in diamond and phosphorus spins in silicon.     

A subfemtotesla multichannel atomic magnetometer

The magnetic field is one of the most fundamental and ubiquitous physical observables, carrying information about all electromagnetic phenomena. For the past 30 years, superconducting quantum interference devices (SQUIDs) operating at 4 K have been unchallenged as ultrahigh-sensitivity magnetic field detectors, with a sensitivity reaching down to 1 fT Hz(-1/2) (1 fT = 10(-15) T). They have enabled, for example, mapping of the magnetic fields produced by the brain, and localization of the underlying electrical activity (magnetoencephalography). Atomic magnetometers, based on detection of Larmor spin precession of optically pumped atoms, have approached similar levels of sensitivity using large measurement volumes, but have much lower sensitivity in the more compact designs required for magnetic imaging applications. Higher sensitivity and spatial resolution combined with non-cryogenic operation of atomic magnetometers would enable new applications, including the possibility of mapping non-invasively the cortical modules in the brain. Here we describe a new spin-exchange relaxation-free (SERF) atomic magnetometer, and demonstrate magnetic field sensitivity of 0.54 fT Hz(-1/2) with a measurement volume of only 0.3 cm3. Theoretical analysis shows that fundamental sensitivity limits of this device are below 0.01 fT Hz(-1/2). We also demonstrate simple multichannel operation of the magnetometer, and localization of magnetic field sources with a resolution of 2 mm.     

Optically programmable electron spin memory using semiconductor quantum dots

The spin of a single electron subject to a static magnetic field provides a natural two-level system that is suitable for use as a quantum bit, the fundamental logical unit in a quantum computer. Semiconductor quantum dots fabricated by strain driven self-assembly are particularly attractive for the realization of spin quantum bits, as they can be controllably positioned, electronically coupled and embedded into active devices. It has been predicted that the atomic-like electronic structure of such quantum dots suppresses coupling of the spin to the solid-state quantum dot environment, thus protecting the 'spin' quantum information against decoherence. Here we demonstrate a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation. We use the device to prepare single electron spins in semiconductor quantum dots with a well defined orientation, and directly measure the intrinsic spin flip time and its dependence on magnetic field. A very long spin lifetime is obtained, with a lower limit of about 20 milliseconds at a magnetic field of 4 tesla and at 1 kelvin.     

Kondo effect in an integer-spin quantum dot

The Kondo effect--a many-body phenomenon in condensed-matter physics involving the interaction between a localized spin and free electrons--was discovered in metals containing small amounts of magnetic impurities, although it is now recognized to be of fundamental importance in a wide class of correlated electron systems. In fabricated structures, the control of single, localized spins is of technological relevance for nanoscale electronics. Experiments have already demonstrated artificial realizations of isolated magnetic impurities at metallic surfaces, nanoscale magnets, controlled transitions between two-electron singlet and triplet states, and a tunable Kondo effect in semiconductor quantum dots. Here we report an unexpected Kondo effect in a few-electron quantum dot containing singlet and triplet spin states, whose energy difference can be tuned with a magnetic field. We observe the effect for an even number of electrons, when the singlet and triplet states are degenerate. The characteristic energy scale is much larger than in the ordinary spin-1/2 case.     

Chemical compass model of avian magnetoreception

Approximately 50 species, including birds, mammals, reptiles, amphibians, fish, crustaceans and insects, are known to use the Earth's magnetic field for orientation and navigation. Birds in particular have been intensively studied, but the biophysical mechanisms that underlie the avian magnetic compass are still poorly understood. One proposal, based on magnetically sensitive free radical reactions, is gaining support despite the fact that no chemical reaction in vitro has been shown to respond to magnetic fields as weak as the Earth's ( approximately 50 muT) or to be sensitive to the direction of such a field. Here we use spectroscopic observation of a carotenoid-porphyrin-fullerene model system to demonstrate that the lifetime of a photochemically formed radical pair is changed by application of < or =50 microT magnetic fields, and to measure the anisotropic chemical response that is essential for its operation as a chemical compass sensor. These experiments establish the feasibility of chemical magnetoreception and give insight into the structural and dynamic design features required for optimal detection of the direction of the Earth's magnetic field.     

Driven coherent oscillations of a single electron spin in a quantum dot

The ability to control the quantum state of a single electron spin in a quantum dot is at the heart of recent developments towards a scalable spin-based quantum computer. In combination with the recently demonstrated controlled exchange gate between two neighbouring spins, driven coherent single spin rotations would permit universal quantum operations. Here, we report the experimental realization of single electron spin rotations in a double quantum dot. First, we apply a continuous-wave oscillating magnetic field, generated on-chip, and observe electron spin resonance in spin-dependent transport measurements through the two dots. Next, we coherently control the quantum state of the electron spin by applying short bursts of the oscillating magnetic field and observe about eight oscillations of the spin state (so-called Rabi oscillations) during a microsecond burst. These results demonstrate the feasibility of operating single-electron spins in a quantum dot as quantum bits.     

Electrical control of spin coherence in semiconductor nanostructures.

The processing of quantum information based on the electron spin degree of freedom requires fast and coherent manipulation of local spins. One approach is to provide spatially selective tuning of the spin splitting--which depends on the g-factor--by using magnetic fields, but this requires their precise control at reduced length scales. Alternative proposals employ electrical gating and spin engineering in semiconductor heterostructures involving materials with different g-factors. Here we show that spin coherence can be controlled in a specially designed AlxGa1-xAs quantum well in which the Al concentration x is gradually varied across the structure. Application of an electric field leads to a displacement of the electron wavefunction within the quantum well, and because the electron g-factor varies strongly with x, the spin splitting is therefore also changed. Using time-resolved optical techniques, we demonstrate gate-voltage-mediated control of coherent spin precession over a 13-GHz frequency range in a fixed magnetic field of 6 T, including complete suppression of precession, reversal of the sign of g, and operation up to room temperature.     

Optical detection of liquid-state NMR

Nuclear magnetic resonance (NMR) in liquids and solids is primarily detected by recording the net dipolar magnetic field outside the spin-polarized sample. But the recorded bulk magnetic field itself provides only limited spatial or structural information about the sample. Most NMR applications rely therefore on more elaborate techniques such as magnetic field gradient encoding or spin correlation spectroscopy, which enable spatially resolved imaging and molecular structure analysis, respectively. Here we demonstrate a fundamentally different and intrinsically information-richer modality of detecting NMR, based on the rotation of the polarization of a laser beam by the nuclear spins in a liquid sample. Optical NMR detection has in fact a long history in atomic vapours with narrow resonance lines, but has so far only been applied to highly specialized condensed matter systems such as quantum dots. It has been predicted that laser illumination can shift NMR frequencies and thus aid detection, but the effect is very small and has never been observed. In contrast, our measurements on water and liquid 129Xe show that the complementary effect-the rotation of light polarization by nuclear spins-is readily measurable, and that it is enhanced dramatically in samples containing heavy nuclei. This approach to optical NMR detection should allow correlated optical and NMR spectroscopy on complex molecules, and continuous two-dimensional imaging of nuclear magnetization with spatial resolution limited only by light diffraction.     

Microwave oscillations of a nanomagnet driven by a spin-polarized current

The recent discovery that a spin-polarized electrical current can apply a large torque to a ferromagnet, through direct transfer of spin angular momentum, offers the possibility of manipulating magnetic-device elements without applying cumbersome magnetic fields. However, a central question remains unresolved: what type of magnetic motions can be generated by this torque? Theory predicts that spin transfer may be able to drive a nanomagnet into types of oscillatory magnetic modes not attainable with magnetic fields alone, but existing measurement techniques have provided only indirect evidence for dynamical states. The nature of the possible motions has not been determined. Here we demonstrate a technique that allows direct electrical measurements of microwave-frequency dynamics in individual nanomagnets, propelled by a d.c. spin-polarized current. We show that spin transfer can produce several different types of magnetic excitation. Although there is no mechanical motion, a simple magnetic-multilayer structure acts like a nanoscale motor; it converts energy from a d.c. electrical current into high-frequency magnetic rotations that might be applied in new devices including microwave sources and resonators.     

Massively parallel manipulation of single cells and microparticles using optical images

The ability to manipulate biological cells and micrometre-scale particles plays an important role in many biological and colloidal science applications. However, conventional manipulation techniques--including optical tweezers, electrokinetic forces (electrophoresis, dielectrophoresis, travelling-wave dielectrophoresis), magnetic tweezers, acoustic traps and hydrodynamic flows--cannot achieve high resolution and high throughput at the same time. Optical tweezers offer high resolution for trapping single particles, but have a limited manipulation area owing to tight focusing requirements; on the other hand, electrokinetic forces and other mechanisms provide high throughput, but lack the flexibility or the spatial resolution necessary for controlling individual cells. Here we present an optical image-driven dielectrophoresis technique that permits high-resolution patterning of electric fields on a photoconductive surface for manipulating single particles. It requires 100,000 times less optical intensity than optical tweezers. Using an incoherent light source (a light-emitting diode or a halogen lamp) and a digital micromirror spatial light modulator, we have demonstrated parallel manipulation of 15,000 particle traps on a 1.3 x 1.0 mm2 area. With direct optical imaging control, multiple manipulation functions are combined to achieve complex, multi-step manipulation protocols.     

Spin-galvanic effect

There is much recent interest in exploiting the spin of conduction electrons in semiconductor heterostructures together with their charge to realize new device concepts. Electrical currents are usually generated by electric or magnetic fields, or by gradients of, for example, carrier concentration or temperature. The electron spin in a spin-polarized electron gas can, in principle, also drive an electrical current, even at room temperature, if some general symmetry requirements are met. Here we demonstrate such a 'spin-galvanic' effect in semiconductor heterostructures, induced by a non-equilibrium, but uniform population of electron spins. The microscopic origin for this effect is that the two electronic sub-bands for spin-up and spin-down electrons are shifted in momentum space and, although the electron distribution in each sub-band is symmetric, there is an inherent asymmetry in the spin-flip scattering events between the two sub-bands. The resulting current flow has been detected by applying a magnetic field to rotate an optically oriented non-equilibrium spin polarization in the direction of the sample plane. In contrast to previous experiments, where spin-polarized currents were driven by electric fields in semiconductor, we have here the complementary situation where electron spins drive a current without the need of an external electric field.     

Optical pumping of a single hole spin in a quantum dot

The spin of an electron is a natural two-level system for realizing a quantum bit in the solid state. For an electron trapped in a semiconductor quantum dot, strong quantum confinement highly suppresses the detrimental effect of phonon-related spin relaxation. However, this advantage is offset by the hyperfine interaction between the electron spin and the 10(4) to 10(6) spins of the host nuclei in the quantum dot. Random fluctuations in the nuclear spin ensemble lead to fast spin decoherence in about ten nanoseconds. Spin-echo techniques have been used to mitigate the hyperfine interaction, but completely cancelling the effect is more attractive. In principle, polarizing all the nuclear spins can achieve this but is very difficult to realize in practice. Exploring materials with zero-spin nuclei is another option, and carbon nanotubes, graphene quantum dots and silicon have been proposed. An alternative is to use a semiconductor hole. Unlike an electron, a valence hole in a quantum dot has an atomic p orbital which conveniently goes to zero at the location of all the nuclei, massively suppressing the interaction with the nuclear spins. Furthermore, in a quantum dot with strong strain and strong quantization, the heavy hole with spin-3/2 behaves as a spin-1/2 system and spin decoherence mechanisms are weak. We demonstrate here high fidelity (about 99 per cent) initialization of a single hole spin confined to a self-assembled quantum dot by optical pumping. Our scheme works even at zero magnetic field, demonstrating a negligible hole spin hyperfine interaction. We determine a hole spin relaxation time at low field of about one millisecond. These results suggest a route to the realization of solid-state quantum networks that can intra-convert the spin state with the polarization of a photon.     

原子自旋共振磁测系统的微波传输优化仿真

对单个电子自旋的研究和控制对于原子陀螺有着极其巨大的潜在应用和科学意义,而氮空位中心(Nitrogen-Vacancy center)作为一个稳定的电子自旋控制体系正在成为一个研究热点。在利用NV中心进行原子陀螺的控制中,微波的传输对于原子陀螺灵敏度具有重要的影响作用。而基于NV中心的原子陀螺系统中高效率的微波照射机构是非常重要的一项。在本文中,我们通过对微波照射机构进行设计,而后利用Comsol软件对微波在SMA探头中的衰减进行仿真,得到了最优化的实验条件,这为后续提高基于NV中心进行原子陀螺的灵敏度奠定了基础。这将对基于NV中心进行原子陀螺系统的开发、磁信息检测具有重要的作用。     

Chiral magnetic order at surfaces driven by inversion asymmetry

Chirality is a fascinating phenomenon that can manifest itself in subtle ways, for example in biochemistry (in the observed single-handedness of biomolecules) and in particle physics (in the charge-parity violation of electroweak interactions). In condensed matter, magnetic materials can also display single-handed, or homochiral, spin structures. This may be caused by the Dzyaloshinskii-Moriya interaction, which arises from spin-orbit scattering of electrons in an inversion-asymmetric crystal field. This effect is typically irrelevant in bulk metals as their crystals are inversion symmetric. However, low-dimensional systems lack structural inversion symmetry, so that homochiral spin structures may occur. Here we report the observation of magnetic order of a specific chirality in a single atomic layer of manganese on a tungsten (110) substrate. Spin-polarized scanning tunnelling microscopy reveals that adjacent spins are not perfectly antiferromagnetic but slightly canted, resulting in a spin spiral structure with a period of about 12 nm. We show by quantitative theory that this chiral order is caused by the Dzyaloshinskii-Moriya interaction and leads to a left-rotating spin cycloid. Our findings confirm the significance of this interaction for magnets in reduced dimensions. Chirality in nanoscale magnets may play a crucial role in spintronic devices, where the spin rather than the charge of an electron is used for data transmission and manipulation. For instance, a spin-polarized current flowing through chiral magnetic structures will exert a spin-torque on the magnetic structure, causing a variety of excitations or manipulations of the magnetization and giving rise to microwave emission, magnetization switching, or magnetic motors.     

Atom-by-atom spectroscopy at graphene edge

The properties of many nanoscale devices are sensitive to local atomic configurations, and so elemental identification and electronic state analysis at the scale of individual atoms is becoming increasingly important. For example, graphene is regarded as a promising candidate for future devices, and the electronic properties of nanodevices constructed from this material are in large part governed by the edge structures. The atomic configurations at graphene boundaries have been investigated by transmission electron microscopy and scanning tunnelling microscopy, but the electronic properties of these edge states have not yet been determined with atomic resolution. Whereas simple elemental analysis at the level of single atoms can now be achieved by means of annular dark field imaging or electron energy-loss spectroscopy, obtaining fine-structure spectroscopic information about individual light atoms such as those of carbon has been hampered by a combination of extremely weak signals and specimen damage by the electron beam. Here we overcome these difficulties to demonstrate site-specific single-atom spectroscopy at a graphene boundary, enabling direct investigation of the electronic and bonding structures of the edge atoms-in particular, discrimination of single-, double- and triple-coordinated carbon atoms is achieved with atomic resolution. By demonstrating how rich chemical information can be obtained from single atoms through energy-loss near-edge fine-structure analysis, our results should open the way to exploring the local electronic structures of various nanodevices and individual molecules.