Matthias Pfender

Nanoscale nuclear magnetic resonance with chemical resolution

NMR on diamonds gets down to chemistry Nuclear magnetic resonance (NMR) spectroscopy is immensely useful for chemical characterization, but it requires relatively large amounts of sample. Recent studies have leveraged nitrogen vacancy centers in diamond to detect NMR signals from samples of just a few cubic nanometers, but with low resolution. Aslam et al. optimized this technique to achieve a resolution of 1 part per million—sufficient to distinguish among alkyl, vinyl, and aryl protons in solution (see the Perspective by Bar-Gill and Retzker). They also demonstrated solid-state implementation and fluorine detection. Science, this issue p. 67; see also p. 38 Nuclear magnetic resonance spectra of miniscule samples via nitrogen vacancies in diamond resolve chemical functionality. Nuclear magnetic resonance (NMR) spectroscopy is a key analytical technique in chemistry, biology, and medicine. However, conventional NMR spectroscopy requires an at least nanoliter-sized sample volume to achieve sufficient signal. We combined the use of a quantum memory and high magnetic fields with a dedicated quantum sensor based on nitrogen vacancy centers in diamond to achieve chemical shift resolution in 1H and 19F NMR spectroscopy of 20-zeptoliter sample volumes. We demonstrate the application of NMR pulse sequences to achieve homonuclear decoupling and spin diffusion measurements. The best measured NMR linewidth of a liquid sample was ~1 part per million, mainly limited by molecular diffusion. To mitigate the influence of diffusion, we performed high-resolution solid-state NMR by applying homonuclear decoupling and achieved a 20-fold narrowing of the NMR linewidth.

Single spin optically detected magnetic resonance with 60–90 GHz (E-band) microwave resonators

Magnetic resonance with ensembles of electron spins is commonly performed around 10 GHz, but also at frequencies above 240 GHz and in corresponding magnetic fields of over 9 T. However, experiments with single electron and nuclear spins so far only reach into frequency ranges of several 10 GHz, where existing coplanar waveguide structures for microwave (MW) delivery are compatible with single spin readout techniques (e.g., electrical or optical readout). Here, we explore the frequency range up to 90 GHz, with magnetic fields of up to ≈3 T for single spin magnetic resonance in conjunction with optical spin readout. To this end, we develop MW resonators with optical single spin access. In our case, rectangular 60-90 GHz (E-band) waveguides guarantee low-loss supply of microwaves to the resonators. Three dimensional cavities, as well as coplanar waveguide resonators, enhance MW fields by spatial and spectral confinement with a MW efficiency of 1.36 mT/√W. We utilize single nitrogen vacancy (NV) centers as hosts for optically accessible spins and show that their properties regarding optical spin readout known from smaller fields (<0.65 T) are retained up to fields of 3 T. In addition, we demonstrate coherent control of single nuclear spins under these conditions. Furthermore, our results extend the applicable magnetic field range of a single spin magnetic field sensor. Regarding spin based quantum registers, high fields lead to a purer product basis of electron and nuclear spins, which promises improved spin lifetimes. For example, during continuous single-shot readout, the (14)N nuclear spin shows second-long longitudinal relaxation times.

Proposal for a room-temperature diamond maser

The application of masers is limited by its demanding working conditions (high vacuum or low temperature). A room-temperature solid-state maser is highly desirable, but the lifetimes of emitters (electron spins) in solids at room temperature are usually too short (∼ns) for population inversion. Masing from pentacene spins in p-terphenyl crystals, which have a long spin lifetime (∼0.1 ms), has been demonstrated. This maser, however, operates only in the pulsed mode. Here we propose a room-temperature maser based on nitrogen-vacancy centres in diamond, which features the longest known solid-state spin lifetime (∼5 ms) at room temperature, high optical pumping efficiency (∼106 s−1) and material stability. Our numerical simulation demonstrates that a maser with a coherence time of approximately minutes is feasible under readily accessible conditions (cavity Q-factor ∼5 × 104, diamond size ∼3 × 3 × 0.5 mm3 and pump power <10 W). A room-temperature diamond maser may facilitate a broad range of microwave technologies.

Single-spin stochastic optical reconstruction microscopy.

Significance Mastering nanoscopic quantum systems promises applications in quantum information processing (QIP) and nanoscale metrology. However, the spatial density of individually addressable systems is not only limited by their size, but rather by the scale needed for control and readout. This affects upscaling of QIP devices and limits nanoscale sensors to be scanning probe devices with serial data acquisition. Here, we simultaneously apply parallel nanoscale microscopy and spin resonance methods on ensembles of optically addressable spins. The latter have been applied as qubits and nanoscale quantum sensors on the single level. In contrast, our method allows parallel individual addressing inside ensembles of qubits/sensors with nanometer distances. This promises a vast speedup for sensing applications compared with scanning probe methods. We experimentally demonstrate precision addressing of single-quantum emitters by combined optical microscopy and spin resonance techniques. To this end, we use nitrogen vacancy (NV) color centers in diamond confined within a few ten nanometers as individually resolvable quantum systems. By developing a stochastic optical reconstruction microscopy (STORM) technique for NV centers, we are able to simultaneously perform sub–diffraction-limit imaging and optically detected spin resonance (ODMR) measurements on NV spins. This allows the assignment of spin resonance spectra to individual NV center locations with nanometer-scale resolution and thus further improves spatial discrimination. For example, we resolved formerly indistinguishable emitters by their spectra. Furthermore, ODMR spectra contain metrology information allowing for sub–diffraction-limit sensing of, for instance, magnetic or electric fields with inherently parallel data acquisition. As an example, we have detected nuclear spins with nanometer-scale precision. Finally, we give prospects of how this technique can evolve into a fully parallel quantum sensor for nanometer resolution imaging of delocalized quantum correlations.

Addressing Single Nitrogen-Vacancy Centers in Diamond with Transparent in-Plane Gate Structures

For many applications of the nitrogen-vacancy (NV) center in diamond, the understanding and active control of its charge state is highly desired. In this work, we demonstrate the reversible manipulation of the charge state of a single NV center from NV(-) across NV(0) to a nonfluorescent, dark state by using an all-diamond in-plane gate nanostructure. Applying a voltage to the in-plane gate structure can influence the energy band bending sufficiently for charge state conversion of NV centers. These diamond in-plane structures can function as transparent top gates, enabling the distant control of the charge state of NV centers tens of micrometers away from the nanostructure.

Nonvolatile nuclear spin memory enables sensor-unlimited nanoscale spectroscopy of small spin clusters

In nanoscale metrology, dissipation of the sensor limits its performance. Strong dissipation has a negative impact on sensitivity, and sensor–target interaction even causes relaxation or dephasing of the latter. The weak dissipation of nitrogen-vacancy (NV) sensors in room temperature diamond enables detection of individual target nuclear spins, yet limits the spectral resolution of nuclear magnetic resonance (NMR) spectroscopy to several hundred Hertz, which typically prevents molecular recognition. Here, we use the NV intrinsic nuclear spin as a nonvolatile classical memory to store NMR information, while suppressing sensor back-action on the target using controlled decoupling of sensor, memory, and target. We demonstrate memory lifetimes up to 4 min and apply measurement and decoupling protocols, which exploit such memories efficiently. Our universal NV-based sensor device records single-spin NMR spectra with 13 Hz resolution at room temperature.Dissipation of the sensor is a limiting factor in metrology. Here, Pfender et al. suppress this effect employing the nuclear spin of an NV centre for robust intermediate storage of classical NMR information, allowing then to record single-spin NMR spectra with 13 Hz resolution at room temperature.

Protecting a Diamond Quantum Memory by Charge State Control

In recent years, solid-state spin systems have emerged as promising candidates for quantum information processing. Prominent examples are the nitrogen-vacancy (NV) center in diamond, phosphorus dopants in silicon (Si:P), rare-earth ions in solids, and VSi-centers in silicon-carbide. The Si:P system has demonstrated that its nuclear spins can yield exceedingly long spin coherence times by eliminating the electron spin of the dopant. For NV centers, however, a proper charge state for storage of nuclear spin qubit coherence has not been identified yet. Here, we identify and characterize the positively charged NV center as an electron-spin-less and optically inactive state by utilizing the nuclear spin qubit as a probe. We control the electronic charge and spin utilizing nanometer scale gate electrodes. We achieve a lengthening of the nuclear spin coherence times by a factor of 4. Surprisingly, the new charge state allows switching of the optical response of single nodes facilitating full individual addressability.

Nuclear quantum-assisted magnetometer

Magnetic sensing and imaging instruments are important tools in biological and material sciences. There is an increasing demand for attaining higher sensitivity and spatial resolution, with implementations using a single qubit offering potential improvements in both directions. In this article we describe a scanning magnetometer based on the nitrogen-vacancy center in diamond as the sensor. By means of a quantum-assisted readout scheme together with advances in photon collection efficiency, our device exhibits an enhancement in signal to noise ratio of close to an order of magnitude compared to the standard fluorescence readout of the nitrogen-vacancy center. This is demonstrated by comparing non-assisted and assisted methods in a T1 relaxation time measurement.