Low-field NMR with multilayer Halbach magnet and NMR selective excitation.

This study introduces a low-field NMR spectrometer (LF-NMR) featuring a multilayer Halbach magnet supported by a combined mechanical and electrical shimming system. This setup offers improved field homogeneity and sensitivity compared to spectrometers relying on typical Halbach and dipole magnets. The multilayer Halbach magnet was designed and assembled using three nested cylindrical magnets, with an additional inner Halbach layer that can be rotated for mechanical shimming. The coils and shim-kernel of the electrical shimming system were constructed and coated with layers of zirconia, thermal epoxy, and silver-paste resin to facilitate passive heat dissipation and ensure mechanical and thermal stability. Furthermore, the 7-channel shim coils were divided into two parts connected in parallel, resulting in a reduction of joule heating temperatures from 96.2 to 32.6 °C. Without the shimming system, the Halbach magnet exhibits a field inhomogeneity of approximately 140 ppm over the sample volume. The probehead was designed to incorporate a solenoidal mini coil, integrated into a single planar board. This design choice aimed to enhance sensitivity, minimize [Formula: see text] inhomogeneity, and reduce impedance discrepancies, transmission loss, and signal reflections. Consequently, the resulting linewidth of water within a 3 mm length and 2.4 mm inner diameter sample volume was 4.5 Hz. To demonstrate the effectiveness of spectral editing in LF-NMR applications at 29.934 MHz, we selectively excited hydroxyl and/or methyl protons in neat acetic acid using optimal control pulses calculated through the Krotov algorithm.

Electron Induced Nanoscale Nuclear Spin Relaxation Probed by Hyperpolarization Injection.

We report on experiments that quantify the role of a central electronic spin as a relaxation source for nuclear spins in its nanoscale environment. Our strategy exploits hyperpolarization injection from the electron as a means to controllably probe an increasing number of nuclear spins in the bath and subsequently interrogate them with high fidelity. Our experiments are focused on a model system of a nitrogen vacancy center electronic spin surrounded by several hundred ^{13}C nuclear spins. We observe that the ^{13}C transverse spin relaxation times vary significantly with the extent of hyperpolarization injection, allowing the ability to measure the influence of electron-mediated relaxation extending over several nanometers. These results suggest interesting new means to spatially discriminate nuclear spins in a nanoscale environment and have direct relevance to dynamic nuclear polarization and quantum sensors and memories constructed from hyperpolarized nuclei.

Variable bandwidth, high efficiency microwave resonator for control of spin-qubits in nitrogen-vacancy centers.

Nitrogen-Vacancy (NV) centers in diamond are attractive tools for sensing and quantum information. Realization of this potential requires effective tools for controlling the spin degree of freedom by microwave (mw) magnetic fields. In this work, we present a planar microwave resonator optimized for microwave-optical double resonance experiments on single NV centers in diamond. It consists of a piece of wide microstrip line, which is symmetrically connected to two 50 Ω microstrip feed lines. In the center of the resonator, an Ω-shaped loop focuses the current and the mw magnetic field. It generates a relatively homogeneous magnetic field over a volume of 0.07 × 0.1 mm3. It can be operated at 2.9 GHz in both transmission and reflection modes with bandwidths of 1000 and 400 MHz, respectively. The high power-to-magnetic field conversion efficiency allows us to produce π-pulses with a duration of 50 ns with only about 200 and 50 mW microwave power in transmission and reflection, respectively. The transmission mode also offers capability for efficient radio frequency excitation. The resonance frequency can be tuned between 1.3 and 6 GHz by adjusting the length of the resonator. This will be useful for experiments on NV-centers at higher external magnetic fields and on different types of optically active spin centers.

Fast Quantum State Tomography in the Nitrogen Vacancy Center of Diamond.

Quantum state tomography is the procedure for reconstructing unknown quantum states from a series of measurements of different observables. Depending on the physical system, different sets of observables have been used for this procedure. In the case of spin qubits, the most common procedure is to measure the transverse magnetization of the system as a function of time. Here, we present a different scheme that relies on time-independent observables and therefore does not require measurements at different evolution times, thereby greatly reducing the overall measurement time. To recover the full density matrix, we use a set of unitary operations that transform the density operator elements into the directly measurable observable. We demonstrate the performance of this scheme in the electron-nuclear spin system of the nitrogen vacancy center in diamond.

Toward the Speed Limit of High-Fidelity Two-Qubit Gates.

Most implementations of quantum gate operations rely on external control fields to drive the evolution of the quantum system. Generating these control fields requires significant efforts to design the suitable control Hamiltonians. Furthermore, any error in the control fields reduces the fidelity of the implemented control operation with respect to the ideal target operation. Achieving sufficiently fast gate operations at low error rates remains therefore a huge challenge. In this Letter, we present a novel approach to overcome this challenge by eliminating, for specific gate operations, the time-dependent control fields entirely. This approach appears useful for maximizing the speed of the gate operation while simultaneously eliminating relevant sources of errors. We present an experimental demonstration of the concept in a single nitrogen-vacancy center in diamond at room temperature.

Floquet Prethermalization with Lifetime Exceeding 90 s in a Bulk Hyperpolarized Solid.

We report the observation of long-lived Floquet prethermal states in a bulk solid composed of dipolar-coupled ^{13}C nuclei in diamond at room temperature. For precessing nuclear spins prepared in an initial transverse state, we demonstrate pulsed spin-lock Floquet control that prevents their decay over multiple-minute-long periods. We observe Floquet prethermal lifetimes T_{2}^{'}≈90.9 s, extended >60 000-fold over the nuclear free induction decay times. The spins themselves are continuously interrogated for ∼10 min, corresponding to the application of ≈5.8×10^{6} control pulses. The ^{13}C nuclei are optically hyperpolarized by lattice nitrogen vacancy centers; the combination of hyperpolarization and continuous spin readout yields significant signal-to-noise ratio in the measurements. This allows probing the Floquet thermalization dynamics with unprecedented clarity. We identify four characteristic regimes of the thermalization process, discerning short-time transient processes leading to the prethermal plateau and long-time system heating toward infinite temperature. This Letter points to new opportunities possible via Floquet control in networks of dilute, randomly distributed, low-sensitivity nuclei. In particular, the combination of minutes-long prethermal lifetimes and continuous spin interrogation opens avenues for quantum sensors constructed from hyperpolarized Floquet prethermal nuclei.

Efficient Implementation of a Quantum Algorithm in a Single Nitrogen-Vacancy Center of Diamond.

Quantum computers have the potential to speed up certain problems that are hard for classical computers. Hybrid systems, such as the nitrogen-vacancy (NV) center in diamond, are among the most promising systems to implement quantum computing, provided the control of the different types of qubits can be efficiently implemented. In the case of the NV center, the anisotropic hyperfine interaction allows one to control the nuclear spins indirectly, through gate operations targeting the electron spin, combined with free precession. Here, we demonstrate that this approach allows one to implement a full quantum algorithm, using the example of Grover's quantum search in a single NV center, whose electron is coupled to a carbon nuclear spin.

Efficient Quantum Gates for Individual Nuclear Spin Qubits by Indirect Control.

Hybrid quantum registers, such as electron-nuclear spin systems, have emerged as promising hardware for implementing quantum information and computing protocols in scalable systems. Nevertheless, the coherent control of such systems still faces challenges. Particularly, the lower gyromagnetic ratios of the nuclear spins cause them to respond slowly to control fields, resulting in gate times that are generally longer than the coherence time of the electron. Here, we demonstrate a scheme for circumventing this problem by indirect control: we apply a small number of short pulses only to the electron and let the full system undergo free evolution under the hyperfine coupling between the pulses. Using this scheme, we realize robust quantum gates in an electron-nuclear spin system, including a Hadamard gate on the nuclear spin and a controlled-NOT gate with the nuclear spin as the target qubit. The durations of these gates are shorter than the electron coherence time, and thus additional operations to extend the system coherence time are not needed. Our demonstration serves as a proof of concept for achieving efficient coherent control of electron-nuclear spin systems, such as nitrogen vacancy centers in diamond. Our scheme is still applicable when the nuclear spins are only weakly coupled to the electron.

Optical detection of magnetic resonance.

The combination of magnetic resonance with laser spectroscopy provides some interesting options for increasing the sensitivity and information content of magnetic resonance. This review covers the basic physics behind the relevant processes, such as angular momentum conservation during absorption and emission. This can be used to enhance the polarization of the spin system by orders of magnitude compared to thermal polarization as well as for detection with sensitivities down to the level of individual spins. These fundamental principles have been used in many different fields. This review summarizes some of the examples in different physical systems, including atomic and molecular systems, dielectric solids composed of rare earth, and transition metal ions and semiconductors.This review was originally written in response to an invitation of "Progress in NMR Spectroscopy" but re-directed to Magnetic Resonance to be accessible to a wide audience. This paper has been reviewed by peers in accordance with the policy of Magnetic Resonance.

Magnetization Dynamics of an Individual Single-Crystalline Fe-Filled Carbon Nanotube.

The magnetization dynamics of individual Fe-filled multiwall carbon-nanotubes (FeCNT), grown by chemical vapor deposition, are investigated by microresonator ferromagnetic resonance (FMR) and Brillouin light scattering (BLS) microscopy and corroborated by micromagnetic simulations. Currently, only static magnetometry measurements are available. They suggest that the FeCNTs consist of a single-crystalline Fe nanowire throughout the length. The number and structure of the FMR lines and the abrupt decay of the spin-wave transport seen in BLS indicate, however, that the Fe filling is not a single straight piece along the length. Therefore, a stepwise cutting procedure is applied in order to investigate the evolution of the ferromagnetic resonance lines as a function of the nanowire length. The results show that the FeCNT is indeed not homogeneous along the full length but is built from 300 to 400 nm long single-crystalline segments. These segments consist of magnetically high quality Fe nanowires with almost the bulk values of Fe and with a similar small damping in relation to thin films, promoting FeCNTs as appealing candidates for spin-wave transport in magnonic applications.

Extending electron paramagnetic resonance to nanoliter volume protein single crystals using a self-resonant microhelix.

Electron paramagnetic resonance (EPR) spectroscopy on protein single crystals is the ultimate method for determining the electronic structure of paramagnetic intermediates at the active site of an enzyme and relating the magnetic tensor to a molecular structure. However, crystals of dimensions typical for protein crystallography (0.05 to 0.3mm) provide insufficient signal intensity. In this work, we present a microwave self-resonant microhelix for nanoliter samples that can be implemented in a commercial X-band (9.5 GHz) EPR spectrometer. The self-resonant microhelix provides a measured signal-to-noise improvement up to a factor of 28 with respect to commercial EPR resonators. This work opens up the possibility to use advanced EPR techniques for studying protein single crystals of dimensions typical for x-ray crystallography. The technique is demonstrated by EPR experiments on single crystal [FeFe]-hydrogenase (Clostridium pasteurianum; CpI) with dimensions of 0.3 mm by 0.1 mm by 0.1 mm, yielding a proposed g-tensor orientation of the Hox state.

Dynamics of frequency-swept nuclear spin optical pumping in powdered diamond at low magnetic fields.

A broad effort is underway to improve the sensitivity of NMR through the use of dynamic nuclear polarization. Nitrogen vacancy (NV) centers in diamond offer an appealing platform because these paramagnetic defects can be optically polarized efficiently at room temperature. However, work thus far has been mainly limited to single crystals, because most polarization transfer protocols are sensitive to misalignment between the NV and magnetic field axes. Here we study the spin dynamics of NV-13C pairs in the simultaneous presence of optical excitation and microwave frequency sweeps at low magnetic fields. We show that a subtle interplay between illumination intensity, frequency sweep rate, and hyperfine coupling strength leads to efficient, sweep-direction-dependent 13C spin polarization over a broad range of orientations of the magnetic field. In particular, our results strongly suggest that finely tuned, moderately coupled nuclear spins are key to the hyperpolarization process, which makes this mechanism distinct from other known dynamic polarization channels. These findings pave the route to applications where powders are intrinsically advantageous, including the hyperpolarization of target fluids in contact with the diamond surface or the use of hyperpolarized particles as contrast agents for in vivo imaging.

Orientation-independent room temperature optical 13C hyperpolarization in powdered diamond.

Dynamic nuclear polarization via contact with electronic spins has emerged as an attractive route to enhance the sensitivity of nuclear magnetic resonance beyond the traditional limits imposed by magnetic field strength and temperature. Among the various alternative implementations, the use of nitrogen vacancy (NV) centers in diamond-a paramagnetic point defect whose spin can be optically polarized at room temperature-has attracted widespread attention, but applications have been hampered by the need to align the NV axis with the external magnetic field. We overcome this hurdle through the combined use of continuous optical illumination and a microwave sweep over a broad frequency range. As a proof of principle, we demonstrate our approach using powdered diamond with which we attain bulk 13C spin polarization in excess of 0.25% under ambient conditions. Remarkably, our technique acts efficiently on diamond crystals of all orientations and polarizes nuclear spins with a sign that depends exclusively on the direction of the microwave sweep. Our work paves the way toward the use of hyperpolarized diamond particles as imaging contrast agents for biosensing and, ultimately, for the hyperpolarization of nuclear spins in arbitrary liquids brought in contact with their surface.

Validation of DWI pre-processing procedures for reliable differentiation between human brain gliomas.

Diffusion magnetic resonance imaging (dMRI) is a powerful tool in clinical applications, in particular, in oncology screening. dMRI demonstrated its benefit and efficiency in the localisation and detection of different types of human brain tumours. Clinical dMRI data suffer from multiple artefacts such as motion and eddy-current distortions, contamination by noise, outliers etc. In order to increase the image quality of the derived diffusion scalar metrics and the accuracy of the subsequent data analysis, various pre-processing approaches are actively developed and used. In the present work we assess the effect of different pre-processing procedures such as a noise correction, different smoothing algorithms and spatial interpolation of raw diffusion data, with respect to the accuracy of brain glioma differentiation. As a set of sensitive biomarkers of the glioma malignancy grades we chose the derived scalar metrics from diffusion and kurtosis tensor imaging as well as the neurite orientation dispersion and density imaging (NODDI) biophysical model. Our results show that the application of noise correction, anisotropic diffusion filtering, and cubic-order spline interpolation resulted in the highest sensitivity and specificity for glioma malignancy grading. Thus, these pre-processing steps are recommended for the statistical analysis in brain tumour studies.

Anisotropic diffusion phantoms based on microcapillaries.

Diffusion MRI is an efficient and widely used technique for the investigation of tissue structure and organisation in vivo. Multiple phenomenological and biophysical diffusion models are intensively exploited for the analysis of the diffusion experiments. However, the verification of the applied diffusion models remains challenging. In order to provide a "gold standard" and to assess the accuracy of the derived parameters and the limitations of the diffusion models, anisotropic diffusion phantoms with well known architecture are demanded. In the present work we built four anisotropic diffusion phantoms consisting of hollow microcapillaries with very small inner diameters of 5, 10 and 20µm and outer diameters of 90 and 150µm. For testing the suitability of these phantoms, we performed diffusion measurements on all of them and evaluated the resulting data with a set of popular diffusion models, such as diffusion tensor and diffusion kurtosis imaging, a two compartment model with intra- and extra-capillary water spaces using bi-exponential fitting, and time-dependent diffusion coefficients in Mitra's limit. The perspectives and limitations of these diffusion phantoms are presented and discussed.

Single-spin magnetic resonance in the nitrogen-vacancy center of diamond.

Magnetic resonance of single spins has flourished mostly because of the unique properties of the NV center in diamond. This review covers the basic physics of this defect center, introduces the techniques for working with single spins and gives an overview of some applications like quantum information and sensing.

Comparative analysis of isotropic diffusion weighted imaging sequences.

Visualisation of living tissue structure and function is a challenging problem of modern imaging techniques. Diffusion MRI allows one to probe in vivo structures on a micrometer scale. However, conventional diffusion measurements are time-consuming procedures, because they require several measurements with different gradient directions. Considerable time savings are therefore possible by measurement schemes that generate an isotropic diffusion weighting in a single shot. Multiple approaches for generating isotropic diffusion weighting are known and have become very popular as useful tools in clinical research. Thus, there is a strong need for a comprehensive comparison of different isotropic weighting approaches. In the present work we introduce two new sequences based on simple (co)sine modulations and compare their performance to established q-space magic-angle spinning sequences and conventional DTI, using a diffusion phantom assembled from microcapillaries and in vivo experiments at 7T. The advantages and disadvantages of all compared schemes are demonstrated and discussed.

Application of the limited-memory quasi-Newton algorithm for multi-dimensional, large flip-angle RF pulses at 7T.

OBJECTIVE: Ultrahigh field MRI provides great opportunities for medical diagnostics and research. However, ultrahigh field MRI also brings challenges, such as larger magnetic susceptibility induced field changes. Parallel-transmit radio-frequency pulses can ameliorate these complications while performing advanced tasks in routine applications. To address one class of such pulses, we propose an optimal-control algorithm as a tool for designing advanced multi-dimensional, large flip-angle, radio-frequency pulses. We contrast initial conditions, constraints, and field correction abilities against increasing pulse trajectory acceleration factors. MATERIALS AND METHODS: On an 8-channel 7T system, we demonstrate the quasi-Newton algorithm with pulse designs for reduced field-of-view imaging with an oil phantom and in vivo with scans of the human brain stem. We used echo-planar imaging with 2D spatial-selective pulses. Pulses are computed sufficiently rapid for routine applications. RESULTS: Our dataset was quantitatively analyzed with the conventional mean-square-error metric and the structural-similarity index from image processing. Analysis of both full and reduced field-of-view scans benefit from utilizing both complementary measures. CONCLUSION: We obtained excellent outer-volume suppression with our proposed method, thus enabling reduced field-of-view imaging using pulse trajectory acceleration factors up to 4.

Measurement with microscopic MRI and simulation of flow in different aneurysm models.

PURPOSE: The impact and the development of aneurysms depend to a significant degree on the exchange of liquid between the regular vessel and the pathological extension. A better understanding of this process will lead to improved prediction capabilities. The aim of the current study was to investigate fluid-exchange in aneurysm models of different complexities by combining microscopic magnetic resonance measurements with numerical simulations. In order to evaluate the accuracy and applicability of these methods, the fluid-exchange process between the unaltered vessel lumen and the aneurysm phantoms was analyzed quantitatively using high spatial resolution. METHODS: Magnetic resonance flow imaging was used to visualize fluid-exchange in two different models produced with a 3D printer. One model of an aneurysm was based on histological findings. The flow distribution in the different models was measured on a microscopic scale using time of flight magnetic resonance imaging. The whole experiment was simulated using fast graphics processing unit-based numerical simulations. The obtained simulation results were compared qualitatively and quantitatively with the magnetic resonance imaging measurements, taking into account flow and spin-lattice relaxation. RESULTS: The results of both presented methods compared well for the used aneurysm models and the chosen flow distributions. The results from the fluid-exchange analysis showed comparable characteristics concerning measurement and simulation. Similar symmetry behavior was observed. Based on these results, the amount of fluid-exchange was calculated. Depending on the geometry of the models, 7% to 45% of the liquid was exchanged per second. CONCLUSIONS: The result of the numerical simulations coincides well with the experimentally determined velocity field. The rate of fluid-exchange between vessel and aneurysm was well-predicted. Hence, the results obtained by simulation could be validated by the experiment. The observed deviations can be caused by the noise in the measurement and by the limited resolution of the simulation. The resulting differences are small enough to allow reliable predictions of the flow distribution in vessels with stents and for pulsed blood flow.

Experimental protection of two-qubit quantum gates against environmental noise by dynamical decoupling.

Hybrid systems consisting of different types of qubits are promising for building quantum computers if they combine useful properties of their constituent qubits. However, they also pose additional challenges if one type of qubits is more susceptible to environmental noise than the others. Dynamical decoupling can help to protect such systems by reducing the decoherence due to the environmental noise, but the protection must be designed such that it does not interfere with the control fields driving the logical operations. Here, we test such a protection scheme on a quantum register consisting of the electronic and nuclear spins of a nitrogen-vacancy center in diamond. The results show that processing is compatible with protection: The dephasing time was extended almost to the limit given by the longitudinal relaxation time of the electron spin.