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.

Ultralong spin coherence time in isotopically engineered diamond.

As quantum mechanics ventures into the world of applications and engineering, materials science faces the necessity to design matter to quantum grade purity. For such materials, quantum effects define their physical behaviour and open completely new (quantum) perspectives for applications. Carbon-based materials are particularly good examples, highlighted by the fascinating quantum properties of, for example, nanotubes or graphene. Here, we demonstrate the synthesis and application of ultrapure isotopically controlled single-crystal chemical vapour deposition (CVD) diamond with a remarkably low concentration of paramagnetic impurities. The content of nuclear spins associated with the (13)C isotope was depleted to 0.3% and the concentration of other paramagnetic defects was measured to be <10(13) cm(-3). Being placed in such a spin-free lattice, single electron spins show the longest room-temperature spin dephasing times ever observed in solid-state systems (T2=1.8 ms). This benchmark will potentially allow observation of coherent coupling between spins separated by a few tens of nanometres, making it a versatile material for room-temperature quantum information processing devices. We also show that single electron spins in the same isotopically engineered CVD diamond can be used to detect external magnetic fields with a sensitivity reaching 4 nT Hz(-1/2) and subnanometre spatial resolution.

Dynamical sensitivity control of a single-spin quantum sensor.

The Nitrogen-Vacancy (NV) defect in diamond is a unique quantum system that offers precision sensing of nanoscale physical quantities at room temperature beyond the current state-of-the-art. The benchmark parameters for nanoscale magnetometry applications are sensitivity, spectral resolution, and dynamic range. Under realistic conditions the NV sensors controlled by conventional sensing schemes suffer from limitations of these parameters. Here we experimentally show a new method called dynamical sensitivity control (DYSCO) that boost the benchmark parameters and thus extends the practical applicability of the NV spin for nanoscale sensing. In contrast to conventional dynamical decoupling schemes, where π pulse trains toggle the spin precession abruptly, the DYSCO method allows for a smooth, analog modulation of the quantum probe's sensitivity. Our method decouples frequency selectivity and spectral resolution unconstrained over the bandwidth (1.85 MHz-392 Hz in our experiments). Using DYSCO we demonstrate high-accuracy NV magnetometry without |2π| ambiguities, an enhancement of the dynamic range by a factor of 4 · 103, and interrogation times exceeding 2 ms in off-the-shelf diamond. In a broader perspective the DYSCO method provides a handle on the inherent dynamics of quantum systems offering decisive advantages for NV centre based applications notably in quantum information and single molecule NMR/MRI.

A nitrogen-vacancy spin based molecular structure microscope using multiplexed projection reconstruction.

Methods and techniques to measure and image beyond the state-of-the-art have always been influential in propelling basic science and technology. Because current technologies are venturing into nanoscopic and molecular-scale fabrication, atomic-scale measurement techniques are inevitable. One such emerging sensing method uses the spins associated with nitrogen-vacancy (NV) defects in diamond. The uniqueness of this NV sensor is its atomic size and ability to perform precision sensing under ambient conditions conveniently using light and microwaves (MW). These advantages have unique applications in nanoscale sensing and imaging of magnetic fields from nuclear spins in single biomolecules. During the last few years, several encouraging results have emerged towards the realization of an NV spin-based molecular structure microscope. Here, we present a projection-reconstruction method that retrieves the three-dimensional structure of a single molecule from the nuclear spin noise signatures. We validate this method using numerical simulations and reconstruct the structure of a molecular phantom ß-cyclodextrin, revealing the characteristic toroidal shape.

Efficient route to high-bandwidth nanoscale magnetometry using single spins in diamond.

Nitrogen-vacancy (NV) center in diamond is a promising quantum metrology tool finding applications across disciplines. The spin sensor measures magnetic fields, electric fields and temperature with nano-scale precision and is fully operable under ambient conditions. Moreover, it achieves precision scaling inversely with total measurement time σB ∝ 1/T (Heisenberg scaling) rather than as the inverse of the square root of T, with σB = √T the Shot-Noise limit. This scaling can be achieved by means of phase estimation algorithms (PEAs), in combination with single-shot read-out. Despite their accuracy, the range of applicability of PEAs is limited to sensing single frequencies with negligible temporal fluctuations. Nuclear Magnetic Resonance (NMR) signals from molecules often contain multifrequency components and sensing them using PEA is ruled out. Here we propose an alternative method for precision magnetometry in frequency multiplexed signals via compressive sensing (CS) techniques focusing on nanoscale NMR. We show that CS can provide for precision scaling approximately as σB ≈ 1/T, as well as for a 5-fold increase in sensitivity over dynamic-range gain, in addition to reducing the total number of resources required. We illustrate our method by taking model solid-state spectra of Glycine acquired under Magic Angle Spinning conditions.

Room temperature high-fidelity holonomic single-qubit gate on a solid-state spin.

At its most fundamental level, circuit-based quantum computation relies on the application of controlled phase shift operations on quantum registers. While these operations are generally compromised by noise and imperfections, quantum gates based on geometric phase shifts can provide intrinsically fault-tolerant quantum computing. Here we demonstrate the high-fidelity realization of a recently proposed fast (non-adiabatic) and universal (non-Abelian) holonomic single-qubit gate, using an individual solid-state spin qubit under ambient conditions. This fault-tolerant quantum gate provides an elegant means for achieving the fidelity threshold indispensable for implementing quantum error correction protocols. Since we employ a spin qubit associated with a nitrogen-vacancy colour centre in diamond, this system is based on integrable and scalable hardware exhibiting strong analogy to current silicon technology. This quantum gate realization is a promising step towards viable, fault-tolerant quantum computing under ambient conditions.

Nitrogen-Vacancy color center in diamond-emerging nanoscale applications in bioimaging and biosensing.

Nitrogen-Vacancy (NV) color center in diamond is a flourishing research area that, in recent years, has displayed remarkable progress. The system offers great potential for realizing futuristic applications in nanoscience, benefiting a range of fields from bioimaging to quantum-sensing. The ability to image single NV color centers in a nanodiamond and manipulate NV electron spin optically under ambient condition is the main driving force behind developments in nanoscale sensing and novel imaging techniques. In this article we discuss current status on the applications of fluorescent nanodiamonds (FND) for optical super resolution nanoscopy, magneto-optical (spin-assisted) sub-wavelength localization and imaging. We present emerging applications such as single molecule spin imaging, nanoscale imaging of biomagnetic fields, sensing molecular fluctuations and temperatures in live cellular environments. We summarize other current advances and future prospects of NV diamond for imaging and sensing pertaining to bio-medical applications.

Highly efficient FRET from a single nitrogen-vacancy center in nanodiamonds to a single organic molecule.

We show highly efficient fluorescence resonance energy transfer (FRET) between negatively charged nitrogen-vacancy (NV) centers in diamond as donor and dye molecules as acceptor, respectively. The energy transfer efficiency is 86% with particles of 20 nm in size. Calculated and experimentally measured energy transfer efficiencies are in excellent agreement. Owing to the small size of the nanocrystals and careful surface preparation, energy transfer between a single nitrogen-vacancy center and a single quencher was identified by the stepwise change of energy transfer efficiencies due to bleaching of single acceptor molecules. Our studies pave the way toward FRET-based scanning probe techniques using single NV donors.

Fluorescence and spin properties of defects in single digit nanodiamonds.

This article reports stable photoluminescence and high-contrast optically detected electron spin resonance (ODESR) from single nitrogen-vacancy (NV) defect centers created within ultrasmall, disperse nanodiamonds of radius less than 4 nm. Unexpectedly, the efficiency for the production of NV fluorescent defects by electron irradiation is found to be independent of the size of the nanocrystals. Fluorescence lifetime imaging shows lifetimes with a mean value of around 17 ns, only slightly longer than the bulk value of the defects. After proper surface cleaning, the dephasing times of the electron spin resonance in the nanocrystals approach values of some microseconds, which is typical for the type Ib diamond from which the nanoparticle is made. We conclude that despite the tiny size of these nanodiamonds the photoactive nitrogen-vacancy color centers retain their bulk properties to the benefit of numerous exciting potential applications in photonics, biomedical labeling, and imaging.