Gopalakrishnan Balasubramanian

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.

Electric-field sensing using single diamond spins.

The ability to sensitively detect charges under amb ient conditions would be a fascinating new tool benefitting a wide range of researchers ac ross disciplines. However, most current techniques are limited to low-temperature methods l ike single-electron transistors (SET)[1,2], single–electron electrostatic force microscopy[3] a nd scanning tunnelling microscopy [4]. Here we open up a new quantum metrology technique demons trating precision electric field measurement using a single nitrogen-vacancy defect entre(NV) spin in diamond. An AC electric field sensitivity reaching ~ 140V/cm/ √Hz has been achieved. This corresponds to the electric field produced by a single elementary char ge located at a distance of ~ 150 nm from our spin sensor with averaging for one second. By caref ul analysis of the electronic structure of the defect centre, we show how an applied magnetic fiel d influences the electric field sensing properties. By this we demonstrate that diamond defct centre spins can be switched between electric and magnetic field sensing modes and ident ify suitable parameter ranges for both detector schemes. By combining magnetic and electri c field sensitivity, nanoscale detection and ambient operation our study opens up new frontiers in imaging and sensing applications ranging from material science to bioimaging.

Quantum register based on coupled electron spins in a room-temperature solid.

Nitrogen–vacancy centres in diamond have emerged as a promising platform for quantum information processing at room temperature. Now, coherent coupling between two electron spins separated by almost 10 nm has been demonstrated. At this distance, the spins can be addressed individually, which might enable the construction of a network of connected quantum registers.

Dynamic Polarization of Single Nuclear Spins by Optical Pumping of Nitrogen-Vacancy Color Centers in Diamond at Room Temperature

We report a versatile method to polarize single nuclear spins in diamond, based on optical pumping of a single nitrogen-vacancy (NV) defect and mediated by a level anticrossing in its excited state. A nuclear-spin polarization higher than 98% is achieved at room temperature for the 15N nuclear spin associated with the NV center, corresponding to microK effective nuclear-spin temperature. We then show simultaneous initialization of two nuclear spins in the vicinity of a NV defect. Such robust control of nuclear-spin states is a key ingredient for further scaling up of nuclear-spin based quantum registers in diamond.

High sensitivity magnetic imaging using an array of spins in diamond.

We present a solid state magnetic field imaging technique using a two-dimensional array of spins in diamond. The magnetic sensing spin array is made of nitrogen vacancy (NV) centers created at shallow depths. Their optical response is used for measuring external magnetic fields in close proximity. Optically detected magnetic resonance is read out from a 60 x 60 microm(2) field of view in a multiplexed manner using a charge coupled device camera. We experimentally demonstrate full two-dimensional vector imaging of the magnetic field produced by a pair of current carrying microwires. The presented wide-field NV magnetometer offers, in addition to its high magnetic sensitivity and vector reconstruction, an unprecedented spatiotemporal resolution and functionality at room temperature.

Excited-state spectroscopy of single NV defects in diamond using optically detected magnetic resonance.

Using pulsed optically detected magnetic resonance techniques, we directly probe electron-spin resonance transitions in the excited-state of single nitrogen-vacancy (NV) color centers in diamond. Unambiguous assignment of excited state fine structure is made, based on changes of NV defect photoluminescence lifetime. This study provides significant insight into the structure of the emitting 3 E excited state, which is invaluable for the development of diamond-based quantum information processing.

Magnetic spin imaging under ambient conditions with sub-cellular resolution.

The detection of small numbers of magnetic spins is a significant challenge in the life, physical and chemical sciences, especially when room temperature operation is required. Here we show that a proximal nitrogen-vacancy spin ensemble serves as a high precision sensing and imaging array. Monitoring its longitudinal relaxation enables sensing of freely diffusing, unperturbed magnetic ions and molecules in a microfluidic device without applying external magnetic fields. Multiplexed charge-coupled device acquisition and an optimized detection scheme permits direct spin noise imaging of magnetically labelled cellular structures under ambient conditions. Within 20 s we achieve spatial resolutions below 500 nm and experimental sensitivities down to 1,000 statistically polarized spins, of which only 32 ions contribute to a net magnetization. The results mark a major step towards versatile sub-cellular magnetic imaging and real-time spin sensing under physiological conditions providing a minimally invasive tool to monitor ion channels or haemoglobin trafficking inside live cells.

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.

Enhanced generation of single optically active spins in diamond by ion implantation

The nitrogen-vacancy (NV) centers in diamond are amongst the most promising candidates for quantum information applications. Up to now the creation of such defects was highly probabilistic, requiring many copies of the nanodevice. Here we show that by employing a two step implantation process which includes low dose N2+ molecular ion implantations followed by high dose C implantation can increase the generation efficiency of NV centers by over 50%. Moreover, we detected intrinsic N14 concentration as low as 0.07 ppb by converting the nitrogen impurities into NV and then counting the single centers by using a confocal microscope.