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The ability to sense and control nuclear spins near solid-state defects might enable a range of quantum technologies. Dynamically Decoupled Radio-Frequency (DDRF) control offers a high degree of design flexibility and long electron-spin coherence times. However, previous studies considered simplified models and little is known about optimal gate design and fundamental limits. Here, we develop a generalised DDRF framework that has important implications for spin sensing and control. Our analytical model, which we corroborate by experiments on a single NV center in diamond, reveals the mechanisms that govern the selectivity of gates and their effective Rabi frequencies, and enables flexible detuned gate designs. We apply these insights to numerically show a 60x sensitivity enhancement for detecting weakly coupled spins and study the optimisation of quantum gates in multi-qubit registers. These results advance the understanding for a broad class of gates and provide a toolbox for application-specific design, enabling improved quantum control and sensing.

Solid-state single-photon emitters provide a versatile platform for exploring quantum technologies such as optically connected quantum networks. A key challenge is to ensure optical coherence and spectral stability of the emitters. Here, we introduce a high-bandwidth `check-probe' scheme to quantitatively measure (laser-induced) spectral diffusion and ionisation rates, as well as homogeneous linewidths. We demonstrate these methods on single V2 centers in commercially available bulk-grown 4H-silicon carbide. Despite observing significant spectral diffusion under laser illumination ($\gtrsim$ GHz/s), the optical transitions are narrow ($\sim$35 MHz), and remain stable in the dark ($\gtrsim$1 s). Through Landau-Zener-St\"uckelberg interferometry, we determine the optical coherence to be near-lifetime limited ($T_2 = 16.4(4)$ ns), hinting at the potential for using bulk-grown materials for developing quantum technologies. These results advance our understanding of spectral diffusion of quantum emitters in semiconductor materials, and may have applications for studying charge dynamics across other platforms.

Solid-state quantum registers consisting of optically active electron spins with nearby nuclear spins are promising building blocks for future quantum technologies. For electron spin-1 registers, dynamical decoupling (DD) quantum gates have been developed that enable the precise control of multiple nuclear spin qubits. However, for the important class of electron spin-1/2 systems, this control method suffers from intrinsic selectivity limitations, resulting in reduced nuclear spin gate fidelities. Here we demonstrate improved control of single nuclear spins by an electron spin-1/2 using Dynamically Decoupled Radio Frequency (DDRF) gates. We make use of the electron spin-1/2 of a diamond tin-vacancy center, showing high-fidelity single-qubit gates, single-shot readout, and spin coherence beyond a millisecond. The DD control is used as a benchmark to observe and control a single carbon-13 nuclear spin. Using the DDRF control method, we demonstrate improved control on that spin. In addition, we find and control an additional nuclear spin that is insensitive to the DD control method. Using these DDRF gates, we show entanglement between the electron and the nuclear spin with 72(3)% state fidelity. Our extensive simulations indicate that DDRF gate fidelities well in excess are feasible. Finally, we employ time-resolved photon detection during readout to quantify the hyperfine coupling for the electron's optically excited state. Our work provides key insights into the challenges and opportunities for nuclear spin control in electron spin-1/2 systems, opening the door to multi-qubit experiments on these promising qubit platforms.

The goal of future quantum networks is to enable new internet applications that are impossible to achieve using solely classical communication. Up to now, demonstrations of quantum network applications and functionalities on quantum processors have been performed in ad-hoc software that was specific to the experimental setup, programmed to perform one single task (the application experiment) directly into low-level control devices using expertise in experimental physics. Here, we report on the design and implementation of the first architecture capable of executing quantum network applications on quantum processors in platform-independent high-level software. We demonstrate the architecture's capability to execute applications in high-level software, by implementing it as a quantum network operating system -- QNodeOS -- and executing test programs including a delegated computation from a client to a server on two quantum network nodes based on nitrogen-vacancy (NV) centers in diamond. We show how our architecture allows us to maximize the use of quantum network hardware, by multitasking different applications on a quantum network for the first time. Our architecture can be used to execute programs on any quantum processor platform corresponding to our system model, which we illustrate by demonstrating an additional driver for QNodeOS for a trapped-ion quantum network node based on a single $^{40}\text{Ca}^+$ atom. Our architecture lays the groundwork for computer science research in the domain of quantum network programming, and paves the way for the development of software that can bring quantum network technology to society., Comment: 12 pages, 5 figures, supplementary materials (48 pages, 24 figures, 11 tables)

Nuclear quadrupolar resonance (NQR) spectroscopy reveals chemical bonding patterns in materials and molecules through the unique coupling between nuclear spins and local fields. However, traditional NQR techniques require macroscopic ensembles of nuclei to yield a detectable signal, which precludes the study of individual molecules and obscures molecule-to-molecule variations due to local perturbations or deformations. Optically active electronic spin qubits, such as the nitrogen-vacancy (NV) center in diamond, facilitate the detection and control of individual nuclei through their local magnetic couplings. Here, we use NV centers to perform NQR spectroscopy on their associated nitrogen-14 ($^{14}$N) nuclei at room temperature. In mapping the nuclear quadrupolar Hamiltonian, we resolve minute variations between individual nuclei. The measurements further reveal correlations between the parameters in the NV center's electronic spin Hamiltonian and the $^{14}$N quadropolar Hamiltonian, as well as a previously unreported Hamiltonian term that results from symmetry breaking. We further design pulse sequences to initialize, readout, and control the quantum evolution of the $^{14}$N nuclear state using the nuclear quadrupolar Hamiltonian., Comment: 15 pages, 10 figures

Spins associated to solid-state colour centers are a promising platform for investigating quantum computation and quantum networks. Recent experiments have demonstrated multi-qubit quantum processors, optical interconnects, and basic quantum error correction protocols. One of the key open challenges towards larger-scale systems is to realize high-fidelity universal quantum gates. In this work, we design and demonstrate a complete high-fidelity gate set for the two-qubit system formed by the electron and nuclear spin of a nitrogen-vacancy center in diamond. We use gate set tomography (GST) to systematically optimise the gates and demonstrate single-qubit gate fidelities of up to $99.999(1)\%$ and a two-qubit gate fidelity of $99.93(5) \%$. Our gates are designed to decouple unwanted interactions and can be extended to other electron-nuclear spin systems. The high fidelities demonstrated provide new opportunities towards larger-scale quantum processing with colour-center qubits.

Perfect-crystal neutron interferometry which is analogous to Mach-Zehnder interferometry, uses Bragg diffraction to form interfering neutron paths. The measured phase shifts can be used to probe many types of interactions whether it be nuclear, electromagnetic, gravitational, or topological in nature. For a perfect-crystal interferometer to preserve coherence, the crystal must possess a high degree of dimensional tolerance as well as being relatively defect-free with minimal internal stresses. In the past, perfect-crystal neutron interferometers have been produced by a two step process. First, a resin diamond wheel would be used to remove excess material and shape the interferometer. Afterword, the crystal would be etched in order to remove surface defects and elevate strains. This process has had limitations in terms of repeatability and in maximizing the final contrast, or fringe visibility, of the interferometer. We have tested various fabrication and post-fabrication techniques on a single perfect-crystal neutron interferometer and measured the interferometer's performance at each step. Here we report a robust, repeatable non-etching fabrication process with high final contrast. For the interferometer used in this work, we achieved contrasts of greater than 90% several separate times and ultimately finished with an interferometer that has 92% contrast and a uniform phase distribution., Comment: 13 Pages, 9 Figures, 1 Table

In the search for scalable, fault-tolerant quantum computing, distributed quantum computers are promising candidates. These systems can be realized in large-scale quantum networks or condensed onto a single chip with closely situated nodes. We present a framework for numerical simulations of a memory channel using the distributed toric surface code, where each data qubit of the code is part of a separate node, and the error-detection performance depends on the quality of four-qubit Greenberger-Horne-Zeilinger (GHZ) states generated between the nodes. We quantitatively investigate the effect of memory decoherence and evaluate the advantage of GHZ creation protocols tailored to the level of decoherence. We do this by applying our framework for the particular case of color centers in diamond, employing models developed from experimental characterization of nitrogen-vacancy centers. For diamond color centers, coherence times during entanglement generation are orders of magnitude lower than coherence times of idling qubits. These coherence times represent a limiting factor for applications, but previous surface code simulations did not treat them as such. Introducing limiting coherence times as a prominent noise factor makes it imperative to integrate realistic operation times into simulations and incorporate strategies for operation scheduling. Our model predicts error probability thresholds for gate and measurement reduced by at least a factor of three compared to prior work with more idealized noise models. We also find a threshold of $4\cdot10^2$ in the ratio between the entanglement generation and the decoherence rates, setting a benchmark for experimental progress., Comment: 24 pages, 13 figures

The field of nanoscale magnetic resonance imaging (NanoMRI) was started 30 years ago. It was motivated by the desire to image single molecules and molecular assemblies, such as proteins and virus particles, with near-atomic spatial resolution and on a length scale of 100 nm. Over the years, the NanoMRI field has also expanded to include the goal of useful high-resolution nuclear magnetic resonance (NMR) spectroscopy of molecules under ambient conditions, including samples up to the micron-scale. The realization of these goals requires the development of spin detection techniques that are many orders of magnitude more sensitive than conventional NMR and MRI, capable of detecting and controlling nanoscale ensembles of spins. Over the years, a number of different technical approaches to NanoMRI have emerged, each possessing a distinct set of capabilities for basic and applied areas of science. The goal of this roadmap article is to report the current state of the art in NanoMRI technologies, outline the areas where they are poised to have impact, identify the challenges that lie ahead, and propose methods to meet these challenges. This roadmap also shows how developments in NanoMRI techniques can lead to breakthroughs in emerging quantum science and technology applications.

The decoherence of a central electron spin due to the dynamics of a coupled electron-spin bath is a core problem in solid-state spin physics. Ensemble experiments have studied the central spin coherence in detail, but such experiments average out the underlying quantum dynamics of the bath. Here, we show the coherent back-action of an individual NV center on an electron-spin bath and use it to detect, prepare and control the dynamics of a pair of bath spins. We image the NV-pair system with sub-nanometer resolution and reveal a long dephasing time ($T_2^* = 44(9)$ ms) for a qubit encoded in the electron-spin pair. Our experiment reveals the microscopic quantum dynamics that underlie the central spin decoherence and provides new opportunities for controlling and sensing interacting spin systems.

Efficient hyperpolarisation of nuclear spins via optically active defect centers, such as the nitrogen vacancy (NV) center in diamond, has great potential for enhancing NMR based quantum information processing and nanoscale magnetic resonance imaging. Recently, pulse-based protocols have been shown to efficiently transfer optically induced polarisation of the electron defect spin to surrounding nuclear spins -- at particular resonant pulse intervals. In this work, we investigate the performance of these protocols, both analytically and experimentally, with the electronic spin of a single NV defect. We find that whenever polarisation resonances of nuclear spins are near-degenerate with a `blocking' spin, which is single spin with stronger off-diagonal coupling to the electronic central spin, they are displaced out of the central resonant region -- without, in general, significant weakening of the resonance. We analyse the underlying physical mechanism and obtain a closed form expression for the displacement. We propose that spin blocking represents a common but overlooked effect in hyperpolarisation of nuclear spins and suggest solutions for improved protocol performance in the presence of (naturally occurring) blocking nuclear spins.

Neutrons have emerged as a unique probe at the forefront of modern material science, unrivaled in their penetrating abilities. A major challenge stems from the fact that neutron optical devices are limited to refractive indices on the order of $n\approx 1 \pm 10^{-5}$. By exploiting advances in precision manufacturing, we have designed and constructed a micro-meter period triangular grating with a high aspect ratio of $14.3$. The manufacturing quality is demonstrated with white-light interferometric data and microscope imaging. Neutron scattering experiment results are presented, showing agreement to refraction modelling. The capabilities of neutron Fresnel lenses based on this design are contrasted to existing neutron focusing techniques and the path separation of a prism-based neutron interferometer is estimated.

Quantum networks can enable long-range quantum communication and modular quantum computation. A powerful approach is to use multi-qubit network nodes which provide the quantum memory and computational power to perform entanglement distillation, quantum error correction, and information processing. Nuclear spins associated with optically-active defects in diamond are promising qubits for this role. However, their dephasing during entanglement distribution across the optical network hinders scaling to larger systems. In this work, we show that a single 13C spin in isotopically engineered diamond offers a long-lived quantum memory that is robust to the optical link operation of an NV centre. The memory lifetime is improved by two orders-of-magnitude upon the state-of-the-art, and exceeds the best reported times for remote entanglement generation. We identify ionisation of the NV centre as a newly limiting decoherence mechanism. As a first step towards overcoming this limitation, we demonstrate that the nuclear spin state can be retrieved with high fidelity after a complete cycle of ionisation and recapture. Finally, we use numerical simulations to show that the combination of this improved memory lifetime with previously demonstrated entanglement links and gate operations can enable key primitives for quantum networks, such as deterministic non-local two-qubit logic operations and GHZ state creation across four network nodes. Our results pave the way for test-bed quantum networks capable of investigating complex algorithms and error correction.

Solid-state spin qubits are a promising platform for quantum computation and quantum networks. Recent experiments have demonstrated high-quality control over multi-qubit systems, elementary quantum algorithms and non-fault-tolerant error correction. Large-scale systems will require using error-corrected logical qubits that are operated fault-tolerantly, so that reliable computation is possible despite noisy operations. Overcoming imperfections in this way remains a major outstanding challenge for quantum science. Here, we demonstrate fault-tolerant operations on a logical qubit using spin qubits in diamond. Our approach is based on the 5-qubit code with a recently discovered flag protocol that enables fault-tolerance using a total of seven qubits. We encode the logical qubit using a novel protocol based on repeated multi-qubit measurements and show that it outperforms non-fault-tolerant encoding schemes. We then fault-tolerantly manipulate the logical qubit through a complete set of single-qubit Clifford gates. Finally, we demonstrate flagged stabilizer measurements with real-time processing of the outcomes. Such measurements are a primitive for fault-tolerant quantum error correction. While future improvements in fidelity and the number of qubits will be required, our realization of fault-tolerant protocols on the logical-qubit level is a key step towards large-scale quantum information processing based on solid-state spins.

The use of the nuclear spins surrounding electron spin qubits as quantum registers and long-lived memories opens the way to new applications in quantum information and biological sensing. Hence, there is a need for generic and robust forms of control of the nuclear registers. Although adiabatic gates are widely used in quantum information, they can become too slow to outpace decoherence. Here, we introduce a technique whereby adiabatic gates arise from the dynamical decoupling protocols that simultaneously extend coherence. We illustrate this pulse-based adiabatic control for nuclear spins around NV centers in diamond. We obtain a closed-form expression from Landau-Zener theory and show that it reliably describes the dynamics. By identifying robust Floquet states, we show that the technique enables polarisation, one-shot flips and state storage for nuclear spins. These results introduce a new control paradigm that combines dynamical decoupling with adiabatic evolution., Comment: 5 pages

The discrete time crystal (DTC) is a recently discovered phase of matter that spontaneously breaks time-translation symmetry. Disorder-induced many-body-localization is required to stabilize a DTC to arbitrary times, yet an experimental investigation of this localized regime has proven elusive. Here, we observe the hallmark signatures of a many-body-localized DTC using a novel quantum simulation platform based on individually controllable $^{13}$C nuclear spins in diamond. We demonstrate the characteristic long-lived spatiotemporal order and confirm that it is robust for generic initial states. Our results are consistent with the realization of an out-of-equilibrium Floquet phase of matter and establish a programmable quantum simulator based on solid-state spins for exploring many-body physics.

Understanding and protecting the coherence of individual quantum systems is a central challenge in quantum science and technology. Over the last decades, a rich variety of methods to extend coherence have been developed. A complementary approach is to look for naturally occurring systems that are inherently protected against decoherence. Here, we show that pairs of identical nuclear spins in solids form intrinsically long-lived quantum systems. We study three carbon-13 pairs in diamond and realize high-fidelity measurements of their quantum states using a single NV center in their vicinity. We then reveal that the spin pairs are robust to external perturbations due to a unique combination of three phenomena: a clock transition, a decoherence-free subspace, and a variant on motional narrowing. The resulting inhomogeneous dephasing time is $T_2^* = 1.9(3)$ minutes, the longest reported for individually controlled qubits. Finally, we develop complete control and realize an entangled state between two spin-pair qubits through projective parity measurements. These long-lived qubits are abundantly present in diamond and other solids, and provide new opportunities for quantum sensing, quantum information processing, and quantum networks.

A promising approach for multi-qubit quantum registers is to use optically addressable spins to control multiple dark electron-spin defects in the environment. While recent experiments have observed signatures of coherent interactions with such dark spins, it is an open challenge to realize the individual control required for quantum information processing. Here we demonstrate the initialisation, control and entanglement of individual dark spins associated to multiple P1 centers, which are part of a spin bath surrounding a nitrogen-vacancy center in diamond. We realize projective measurements to prepare the multiple degrees of freedom of P1 centers - their Jahn-Teller axis, nuclear spin and charge state - and exploit these to selectively access multiple P1s in the bath. We develop control and single-shot readout of the nuclear and electron spin, and use this to demonstrate an entangled state of two P1 centers. These results provide a proof-of-principle towards using dark electron-nuclear spin defects as qubits for quantum sensing, computation and networks.

The neutral charge state plays an important role in quantum information and sensing applications based on nitrogen-vacancy centers. However, the orbital and spin dynamics remain unexplored. Here, we use resonant excitation of single centers to directly reveal the fine structure, enabling selective addressing of spin-orbit states. Through pump-probe experiments, we find the orbital relaxation time (430ns at 4.7K) and measure its temperature-dependence up to 11.8K. Finally we reveal the spin relaxation time (1.5s), and realize projective high-fidelity single-shot readout of the spin state ($\geq98\%$)., Comment: 14 pages, 10 figures (incl. Supplemental Material)

The detection of nuclear spins using individual electron spins has enabled new opportunities in quantum sensing and quantum information processing. Proof-of-principle experiments have demonstrated atomic-scale imaging of nuclear-spin samples and controlled multi-qubit registers. However, to image more complex samples and to realize larger-scale quantum processors, computerized methods that efficiently and automatically characterize spin systems are required. Here, we realize a deep learning model for automatic identification of nuclear spins using the electron spin of single nitrogen-vacancy (NV) centers in diamond as a sensor. Based on neural network algorithms, we develop noise recovery procedures and training sequences for highly non-linear spectra. We apply these methods to experimentally demonstrate fast identification of 31 nuclear spins around a single NV center and accurately determine the hyperfine parameters. Our methods can be extended to larger spin systems and are applicable to a wide range of electron-nuclear interaction strengths. These results enable efficient imaging of complex spin samples and automatic characterization of large spin-qubit registers.

Efficiently detecting and characterizing individual spins in solid-state hosts is an essential step to expand the fields of quantum sensing and quantum information processing. While selective detection and control of a few 13C nuclear spins in diamond have been demonstrated using the electron spin of nitrogen-vacancy (NV) centers, a reliable, efficient, and automatic characterization method is desired. Here, we develop an automated algorithmic method for decomposing spectral data to identify and characterize multiple nuclear spins in diamond. We demonstrate efficient nuclear spin identification and accurate reproduction of hyperfine interaction components for both virtual and experimental nuclear spectroscopy data. We conduct a systematic analysis of this methodology and discuss the range of hyperfine interaction components of each nuclear spin that the method can efficiently detect. The result demonstrates a systematic approach that automatically detects nuclear spins with the aid of computational methods, facilitating the future scalability of devices., Comment: 4 figures, 2 tables

Nuclear magnetic resonance (NMR) is a powerful method for determining the structure of molecules and proteins. While conventional NMR requires averaging over large ensembles, recent progress with single-spin quantum sensors has created the prospect of magnetic imaging of individual molecules. As an initial step towards this goal, isolated nuclear spins and spin pairs have been mapped. However, large clusters of interacting spins - such as found in molecules - result in highly complex spectra. Imaging these complex systems is an outstanding challenge due to the required high spectral resolution and efficient spatial reconstruction with sub-angstrom precision. Here we develop such atomic-scale imaging using a single nitrogen-vacancy (NV) centre as a quantum sensor, and demonstrate it on a model system of $27$ coupled $^{13}$C nuclear spins in a diamond. We present a new multidimensional spectroscopy method that isolates individual nuclear-nuclear spin interactions with high spectral resolution ($< 80\,$mHz) and high accuracy ($2$ mHz). We show that these interactions encode the composition and inter-connectivity of the cluster, and develop methods to extract the 3D structure of the cluster with sub-angstrom resolution. Our results demonstrate a key capability towards magnetic imaging of individual molecules and other complex spin systems.

Spins associated to single defects in solids provide promising qubits for quantum information processing and quantum networks. Recent experiments have demonstrated long coherence times, high-fidelity operations and long-range entanglement. However, control has so far been limited to a few qubits, with entangled states of three spins demonstrated. Realizing larger multi-qubit registers is challenging due to the need for quantum gates that avoid crosstalk and protect the coherence of the complete register. In this paper, we present novel decoherence-protected gates that combine dynamical decoupling of an electron spin with selective phase-controlled driving of nuclear spins. We use these gates to realize a 10-qubit quantum register consisting of the electron spin of a nitrogen-vacancy center and 9 nuclear spins in diamond. We show that the register is fully connected by generating entanglement between all 45 possible qubit pairs, and realize genuine multipartite entangled states with up to 7 qubits. Finally, we investigate the register as a multi-qubit memory. We show coherence times up to 63(2) seconds - the longest reported for a single solid-state qubit - and demonstrate that two-qubit entangled states can be stored for over 10 seconds. Our results enable the control of large quantum registers with long coherence times and therefore open the door to advanced quantum algorithms and quantum networks with solid-state spin qubits.

Spin-orbit coupling of light has come to the fore in nano-optics and plasmonics, and is a key ingredient of topological photonics and chiral quantum optics. We demonstrate a basic tool for incorporating analogous effects into neutron optics: the generation and detection of neutron beams with coupled spin and orbital angular momentum. $^3$He neutron spin-filters are used in conjunction with specifically oriented triangular coils to prepare neutron beams with lattices of spin-orbit correlations, as demonstrated by their spin-dependant intensity profiles. These correlations can be tailored to particular applications, such as neutron studies of topological materials.

We report on the realization and application of non-destructive three-qubit parity measurements on nuclear spin qubits in diamond. We use high-fidelity quantum logic to map the parity of the joint state of three nuclear spin qubits onto an electronic spin qubit that acts as an ancilla, followed by single-shot non-destructive readout of the ancilla combined with an electron spin echo to ensure outcome-independent evolution of the nuclear spins. Through the sequential application of three such parity measurements, we demonstrate the generation of genuine multipartite entangled states out of the maximally mixed state. Furthermore, we implement a single-shot version of the GHZ experiment that can generate a quantum versus classical contradiction in each run. Finally, we test a state-independent non-contextuality inequality in eight dimensions. The techniques and insights developed here are relevant for fundamental tests as well as for quantum information protocols such as quantum error correction.

The advancement of quantum optical science and technology with solid-state emitters such as nitrogen-vacancy (NV) centers in diamond critically relies on the coherence of the emitters' optical transitions. A widely employed strategy to create NV centers at precisely controlled locations is nitrogen ion implantation followed by a high-temperature annealing process. We report on experimental data directly correlating the NV center optical coherence to the origin of the nitrogen atom. These studies reveal low-strain, narrow-optical-linewidth ($<500$ MHz) NV centers formed from naturally-occurring $^{14}$N atoms. In contrast, NV centers formed from implanted $^{15}$N atoms exhibit significantly broadened optical transitions ($>1$ GHz) and higher strain. The data show that the poor optical coherence of the NV centers formed from implanted nitrogen is not due to an intrinsic effect related to the diamond or isotope. These results have immediate implications for the positioning accuracy of current NV center creation protocols and point to the need to further investigate the influence of lattice damage on the coherence of NV centers from implanted ions.

We describe an experimental protocol to characterize magnetic field dependent microwave losses in superconducting niobium microstrip resonators. Our approach provides a unified view that covers two well-known magnetic field dependent loss mechanisms: quasiparticle generation and vortex motion. We find that quasiparticle generation is the dominant loss mechanism for parallel magnetic fields. For perpendicular fields, the dominant loss mechanism is vortex motion or switches from quasiparticle generation to vortex motion, depending on cooling procedures. In particular, we introduce a plot of the quality factor versus the resonance frequency as a general method for identifying the dominant loss mechanism. We calculate the expected resonance frequency and the quality factor as a function of the magnetic field by modeling the complex resistivity. Key parameters characterizing microwave loss are estimated from comparisons of the observed and expected resonator properties. Based on these key parameters, we find a niobium resonator whose thickness is similar to its penetration depth is the best choice for X-band electron spin resonance applications. Finally, we detect partial release of the Meissner current at the vortex penetration field, suggesting that the interaction between vortices and the Meissner current near the edges is essential to understand the magnetic field dependence of the resonator properties.

Single electron spins coupled to multiple nuclear spins provide promising multi-qubit registers for quantum sensing and quantum networks. The obtainable level of control is determined by how well the electron spin can be selectively coupled to, and decoupled from, the surrounding nuclear spins. Here we realize a coherence time exceeding a second for a single electron spin through decoupling sequences tailored to its microscopic nuclear-spin environment. We first use the electron spin to probe the environment, which is accurately described by seven individual and six pairs of coupled carbon-13 spins. We develop initialization, control and readout of the carbon-13 pairs in order to directly reveal their atomic structure. We then exploit this knowledge to store quantum states for over a second by carefully avoiding unwanted interactions. These results provide a proof-of-principle for quantum sensing of complex multi-spin systems and an opportunity for multi-qubit quantum registers with long coherence times.