Spins associated to optically accessible solid-state defects have emerged as a versatile platform for exploring quantum simulation, quantum sensing and quantum communication. Pioneering experiments have shown the sensing, imaging, and control of multiple nuclear spins surrounding a single electron spin defect. However, the accessible size of these spin networks has been constrained by the spectral resolution of current methods. Here, we map a network of 50 coupled spins through high-resolution correlated sensing schemes, using a single nitrogen-vacancy center in diamond. We develop concatenated double-resonance sequences that identify spin-chains through the network. These chains reveal the characteristic spin frequencies and their interconnections with high spectral resolution, and can be fused together to map out the network. Our results provide new opportunities for quantum simulations by increasing the number of available spin qubits. Additionally, our methods might find applications in nano-scale imaging of complex spin systems external to the host crystal.

Solid-state spin qubits is a promising platform for quantum computation and quantum networks^1,2. Recent experiments have demonstrated high-quality control over multi-qubit systems^3–8, elementary quantum algorithms^8–11 and non-fault-tolerant error correction^12–14. Large-scale systems will require using error-corrected logical qubits that are operated fault tolerantly, so that reliable computation becomes possible despite noisy operations^15–18. Overcoming imperfections in this way remains an important outstanding challenge for quantum science^15,19–27. Here, we demonstrate fault-tolerant operations on a logical qubit using spin qubits in diamond. Our approach is based on the five-qubit code with a recently discovered flag protocol that enables fault tolerance using a total of seven qubits^28–30. We encode the logical qubit using a new 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. Although future improvements in fidelity and the number of qubits will be required to suppress logical error rates below the physical error rates, our realization of fault-tolerant protocols on the logical-qubit level is a key step towards 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 polarization, one-shot flips, and state storage for nuclear spins. These results introduce a control paradigm that combines dynamical decoupling with adiabatic evolution.

Understanding and protecting the coherence of individual quantum systems is a central challenge in quantum science and technology. Over the past 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 qubits. We study three carbon-13 pairs in diamond and realize high-fidelity measurements of their quantum states using a single nitrogen-vacancy center in their vicinity. We then reveal that the spin pairs are robust to external perturbations due to a combination of three phenomena: a decoherence-free subspace, a clock transition, and a variant on motional narrowing. The resulting inhomogeneous dephasing time is T2∗=1.9(3) min, the longest reported for individually controlled qubits. Finally, we develop complete control and realize an entangled state between two spin pairs through projective parity measurements. These long-lived qubits are abundantly present in diamond and other solids and provide new opportunities for ancilla-enhanced quantum sensing and for robust memory qubits for quantum networks.

The discrete time crystal (DTC) is a nonequilibrium phase of matter that spontaneously breaks timetranslation symmetry. Disorder-induced many-body localization can stabilize the DTC phase by breaking ergodicity and preventing thermalization. Here, we observe the hallmark signatures of the manybody- localized DTC using a quantum simulation platform based on individually controllable carbon-13 nuclear spins in diamond. We demonstrate long-lived period-doubled oscillations and confirm that they are robust for generic initial states, thus showing the characteristic time-crystalline order across the many-body spectrum. Our results are consistent with the realization of an out-of-equilibrium Floquet phase of matter and introduce a programmable quantum simulator based on solid-state spins for exploring many-body physics.

Nuclear magnetic resonance (NMR) is a powerful method for determining the structure of molecules and proteins¹. Whereas conventional NMR requires averaging over large ensembles, recent progress with single-spin quantum sensors^2–9 has created the prospect of magnetic imaging of individual molecules^10–13. As an initial step towards this goal, isolated nuclear spins and spin pairs have been mapped^14–21. However, large clusters of interacting spins—such as those found in molecules—result in highly complex spectra. Imaging these complex systems is challenging because it requires high spectral resolution and efficient spatial reconstruction with sub-ångström precision. Here we realize such atomic-scale imaging using a single nitrogen vacancy centre as a quantum sensor, and demonstrate it on a model system of 27 coupled ¹³C nuclear spins in diamond. We present a multidimensional spectroscopy method that isolates individual nuclear–nuclear spin interactions with high spectral resolution (less than 80 millihertz) and high accuracy (2 millihertz). We show that these interactions encode the composition and inter-connectivity of the cluster, and develop methods to extract the three-dimensional structure of the cluster with sub-ångström resolution. Our results demonstrate a key capability towards magnetic imaging of individual molecules and other complex spin systems^9–13.

Spins associated with 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 multiqubit registers is challenging due to the need for quantum gates that avoid cross talk 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 ten-qubit quantum register consisting of the electron spin of a nitrogen-vacancy center and nine 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 seven qubits. Finally, we investigate the register as a multiqubit memory. We demonstrate the protection of an arbitrary single-qubit state for over 75 s-the longest reported for a single solid-state qubit-and show that two-qubit entanglement can be preserved for over 10 s. 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.