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.     

Nanoscale magnetic sensing with an individual electronic spin in diamond

Detection of weak magnetic fields with nanoscale spatial resolution is an outstanding problem in the biological and physical sciences. For example, at a distance of 10 nm, the spin of a single electron produces a magnetic field of about 1 muT, and the corresponding field from a single proton is a few nanoteslas. A sensor able to detect such magnetic fields with nanometre spatial resolution would enable powerful applications, ranging from the detection of magnetic resonance signals from individual electron or nuclear spins in complex biological molecules to readout of classical or quantum bits of information encoded in an electron or nuclear spin memory. Here we experimentally demonstrate an approach to such nanoscale magnetic sensing, using coherent manipulation of an individual electronic spin qubit associated with a nitrogen-vacancy impurity in diamond at room temperature. Using an ultra-pure diamond sample, we achieve detection of 3 nT magnetic fields at kilohertz frequencies after 100 s of averaging. In addition, we demonstrate a sensitivity of 0.5 muT Hz(-1/2) for a diamond nanocrystal with a diameter of 30 nm.     

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.     

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.     

Electronic read-out of a single nuclear spin using a molecular spin transistor

Quantum control of individual spins in condensed-matter devices is an emerging field with a wide range of applications, from nanospintronics to quantum computing. The electron, possessing spin and orbital degrees of freedom, is conventionally used as the carrier of quantum information in proposed devices. However, electrons couple strongly to the environment, and so have very short relaxation and coherence times. It is therefore extremely difficult to achieve quantum coherence and stable entanglement of electron spins. Alternative concepts propose nuclear spins as the building blocks for quantum computing, because such spins are extremely well isolated from the environment and less prone to decoherence. However, weak coupling comes at a price: it remains challenging to address and manipulate individual nuclear spins. Here we show that the nuclear spin of an individual metal atom embedded in a single-molecule magnet can be read out electronically. The observed long lifetimes (tens of seconds) and relaxation characteristics of nuclear spin at the single-atom scale open the way to a completely new world of devices in which quantum logic may be implemented.     

Triplet-singlet spin relaxation via nuclei in a double quantum dot

The spin of a confined electron, when oriented originally in some direction, will lose memory of that orientation after some time. Physical mechanisms leading to this relaxation of spin memory typically involve either coupling of the electron spin to its orbital motion or to nuclear spins. Relaxation of confined electron spin has been previously measured only for Zeeman or exchange split spin states, where spin-orbit effects dominate relaxation; spin flips due to nuclei have been observed in optical spectroscopy studies. Using an isolated GaAs double quantum dot defined by electrostatic gates and direct time domain measurements, we investigate in detail spin relaxation for arbitrary splitting of spin states. Here we show that electron spin flips are dominated by nuclear interactions and are slowed by several orders of magnitude when a magnetic field of a few millitesla is applied. These results have significant implications for spin-based information processing.     

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.     

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.     

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.     

动力学去耦提升N@C_（60）@C_（60）H_（28）单晶中电子自旋相干时间的实验研究

内嵌富勒烯N@C60与C60H28分子共结晶形成的单晶N@C60@C60H28,能够实现N@C60的有序排列,从而在实现基于内嵌富勒烯的可扩展量子计算上具有着突出的潜力.本项研究中,我们对单晶N@C60@C60H28中氮电子自旋的弛豫时间和弛豫机制做了详细的测试和分析,厘清了N@C60@C60H28样品中氮电子自旋相干时间（T2）降低的主要原因来自C60H28分子中质子核自旋热库的影响.通过动力学去耦实验技术,我们进一步有效地抑制了这一不利影响,实现了氮电子自旋T2时间的显著提升.这一研究结果对于更好地保护编码于有序富勒烯内电子自旋上的量子信息,进而实现量子计算,具有重要的意义.     

Electron tomography at 2.4-ångström resolution

Transmission electron microscopy is a powerful imaging tool that has found broad application in materials science, nanoscience and biology. With the introduction of aberration-corrected electron lenses, both the spatial resolution and the image quality in transmission electron microscopy have been significantly improved and resolution below 0.5??ngstr?ms has been demonstrated. To reveal the three-dimensional (3D) structure of thin samples, electron tomography is the method of choice, with cubic-nanometre resolution currently achievable. Discrete tomography has recently been used to generate a 3D atomic reconstruction of a silver nanoparticle two to three nanometres in diameter, but this statistical method assumes prior knowledge of the particle's lattice structure and requires that the atoms fit rigidly on that lattice. Here we report the experimental demonstration of a general electron tomography method that achieves atomic-scale resolution without initial assumptions about the sample structure. By combining a novel projection alignment and tomographic reconstruction method with scanning transmission electron microscopy, we have determined the 3D structure of an approximately ten-nanometre gold nanoparticle at 2.4-?ngstr?m resolution. Although we cannot definitively locate all of the atoms inside the nanoparticle, individual atoms are observed in some regions of the particle and several grains are identified in three dimensions. The 3D surface morphology and internal lattice structure revealed are consistent with a distorted icosahedral multiply twinned particle. We anticipate that this general method can be applied not only to determine the 3D structure of nanomaterials at atomic-scale resolution, but also to improve the spatial resolution and image quality in other tomography fields.     

纳米级自旋分离的铁磁共振成像研究

自旋间的相互作用力对原子级别纳米构造体磁性质的理解是极为重要的.磁交换力显微镜(MExFM)是测量原子磁矩相互作用力的一种创新手段,但是这种手段不能分离表面形貌和自旋信息.我们提出的铁磁共振磁交换力显微镜(FMR-MExFM)实现了磁性材料表面的磁交换力信息和表面形貌信息的分离.为了充分利用铁磁共振效应,高效率的微波照射机构是极为重要的一项.在本研究中,通过照射机构的仿真和优化设计得到了微波在同轴电缆间的衰减、照射机构直径以及同轴电缆-探针距离之间的关系,同时得到了最优化的实验条件,在此基础上提高了铁磁共振检测的灵敏度.运用改进后的FMR-MExFM,成功地完全分离了磁性信息和表面结构信息,实现了磁性信息N极和S极的180°的相位差.本研究对FMR-MExFM的开发、磁信息检测具有重要的作用.     

Controlled multiple quantum coherences of nuclear spins in a nanometre-scale device

The analytical technique of nuclear magnetic resonance (NMR) is based on coherent quantum mechanical superposition of nuclear spin states. Recently, NMR has received considerable renewed interest in the context of quantum computation and information processing, which require controlled coherent qubit operations. However, standard NMR is not suitable for the implementation of realistic scalable devices, which would require all-electrical control and the means to detect microscopic quantities of coherent nuclear spins. Here we present a self-contained NMR semiconductor device that can control nuclear spins in a nanometre-scale region. Our approach enables the direct detection of (otherwise invisible) multiple quantum coherences between levels separated by more than one quantum of spin angular momentum. This microscopic high sensitivity NMR technique is especially suitable for probing materials whose nuclei contain multiple spin levels, and may form the basis of a versatile multiple qubit device.     

Magnetic exchange force microscopy with atomic resolution

The ordering of neighbouring atomic magnetic moments (spins) leads to important collective phenomena such as ferromagnetism and antiferromagnetism. A full understanding of magnetism on the nanometre scale therefore calls for information on the arrangement of spins in real space and with atomic resolution. Spin-polarized scanning tunnelling microscopy accomplishes this but can probe only conducting materials. Force microscopy can be used on any sample independent of its conductivity. In particular, magnetic force microscopy is well suited to exploring ferromagnetic domain structures. However, atomic resolution cannot be achieved because data acquisition involves the sensing of long-range magnetostatic forces between tip and sample. Magnetic exchange force microscopy has been proposed for overcoming this limitation: by using an atomic force microscope with a magnetic tip, it should be possible to detect the short-range magnetic exchange force between tip and sample spins. Here we show for a prototypical antiferromagnetic insulator, the (001) surface of nickel oxide, that magnetic exchange force microscopy can indeed reveal the arrangement of both surface atoms and their spins simultaneously. In contrast with previous attempts to implement this method, we use an external magnetic field to align the magnetic polarization at the tip apex so as to optimize the interaction between tip and sample spins. This allows us to observe the direct magnetic exchange coupling between the spins of the tip atom and sample atom that are closest to each other, and thereby demonstrate the potential of magnetic exchange force microscopy for investigations of inter-spin interactions at the atomic level.     

Emergent excitations in a geometrically frustrated magnet

Frustrated systems are ubiquitous, and they are interesting because their behaviour is difficult to predict; frustration can lead to macroscopic degeneracies and qualitatively new states of matter. Magnetic systems offer good examples in the form of spin lattices, where all interactions between spins cannot be simultaneously satisfied. Here we report how unusual composite spin degrees of freedom can emerge from frustrated magnetic interactions in the cubic spinel ZnCr(2)O(4). Upon cooling, groups of six spins self-organize into weakly interacting antiferromagnetic loops, whose directors -- the unique direction along which the spins are aligned, parallel or antiparallel -- govern all low-temperature dynamics. The experimental evidence comes from a measurement of the magnetic form factor by inelastic neutron scattering; the data show that neutrons scatter from hexagonal spin clusters rather than individual spins. The hexagon directors are, to a first approximation, decoupled from each other, and hence their reorientations embody the long-sought local zero energy modes for the pyrochlore lattice.     

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.     

Tomographic imaging using the nonlinear response of magnetic particles

The use of contrast agents and tracers in medical imaging has a long history. They provide important information for diagnosis and therapy, but for some desired applications, a higher resolution is required than can be obtained using the currently available medical imaging techniques. Consider, for example, the use of magnetic tracers in magnetic resonance imaging: detection thresholds for in vitro and in vivo imaging are such that the background signal from the host tissue is a crucial limiting factor. A sensitive method for detecting the magnetic particles directly is to measure their magnetic fields using relaxometry; but this approach has the drawback that the inverse problem (associated with transforming the data into a spatial image) is ill posed and therefore yields low spatial resolution. Here we present a method for obtaining a high-resolution image of such tracers that takes advantage of the nonlinear magnetization curve of small magnetic particles. Initial 'phantom' experiments are reported that demonstrate the feasibility of the imaging method. The resolution that we achieve is already well below 1 mm. We evaluate the prospects for further improvement, and show that the method has the potential to be developed into an imaging method characterized by both high spatial resolution as well as high sensitivity.     

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.     

Minority spin condensate in the spin-polarized superfluid 3He A1 phase

The magnetic properties of (3)He in its various phases originate from the interactions among the nuclear spins. The spin-polarized 'ferromagnetic' superfluid (3)He A(1) phase (which forms below 3 mK between two transition temperatures, T(c1) and T(c2), in an external magnetic field) serves as a material in which theories of fundamental magnetic processes and macroscopic quantum spin phenomena may be tested. Conventionally, the superfluid component of the A(1) phase is understood to contain only the majority spin condensate, having energetically favoured paired spins directed along the external field and no minority spin condensate having paired spins in the opposite direction. Because of difficulties in satisfying both the ultralow temperature and high magnetic field required to produce a substantial phase space, there exist few studies of spin dynamics phenomena that could be used to test the conventional view of the A(1) phase. Here we develop a mechanical spin density detector that operates in the required regime, enabling us to perform measurements of spin relaxation in the A(1) phase as a function of temperature, pressure and magnetic field. Our mechanical spin detector is based in principle on the magnetic fountain effect; spin-polarized superfluid motion can be induced both magnetically and mechanically, and we demonstrate the feasibility of increasing spin polarization by a mechanical spin filtering process. In the high temperature range of the A(1) phase near T(c1), the measured spin relaxation time is long, as expected. Unexpectedly, the spin relaxation rate increases rapidly as the temperature is decreased towards T(c2). Our measurements, together with Leggett-Takagi theory, demonstrate that a minute presence of minority spin pairs is responsible for this unexpected spin relaxation behaviour. Thus, the long-held conventional view that the A(1) phase contains only the majority spin condensate is inadequate.     

基于Gd的造影剂在T1加权MRI上的研究进展

磁共振成像(MRI)由于具有较深的组织穿透能力和高的空间分辨率,已成为临床医学常规使用的诊断工具之一.MRI造影剂能有效提高病灶区域和周围组织的对比度,被广泛应用于MRI医疗诊断.基于Gd的MRI造影剂,由于其能最大程度地加速纵向弛豫,产生更明亮的图像,使得该类造影剂被科研工作者不断开发和研究.综述了Gd造影剂在T1加权MRI上的最新研究进展.