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.

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.

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 heralded 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 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.

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.

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.

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 nitrogen-vacancy electron spin through decoupling sequences tailored to its microscopic nuclear-spin environment. First, we 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 in the electron spin 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.

Large-scale quantum networks promise to enable secure communication, distributed quantum computing, enhanced sensing and fundamental tests of quantum mechanics through the distribution of entanglement across nodes ^1-7. Moving beyond current two-node networks ^8-13 requires the rate of entanglement generation between nodes to exceed the decoherence (loss) rate of the entanglement. If this criterion is met, intrinsically probabilistic entangling protocols can be used to provide deterministic remote entanglement at pre-specified times. Here we demonstrate this using diamond spin qubit nodes separated by two metres. We realize a fully heralded single-photon entanglement protocol that achieves entangling rates of up to 39 hertz, three orders of magnitude higher than previously demonstrated two-photon protocols on this platform ¹⁴. At the same time, we suppress the decoherence rate of remote-entangled states to five hertz through dynamical decoupling. By combining these results with efficient charge-state control and mitigation of spectral diffusion, we deterministically deliver a fresh remote state with an average entanglement fidelity of more than 0.5 at every clock cycle of about 100 milliseconds without any pre-or post-selection. These results demonstrate a key building block for extended quantum networks and open the door to entanglement distribution across multiple remote nodes.

The impact of future quantum networks hinges on high-quality quantum entanglement shared between network nodes. Unavoidable imperfections necessitate a means to improve remote entanglement by local quantum operations. We realize entanglement distillation on a quantum network primitive of distant electron-nuclear two-qubit nodes. The heralded generation of two copies of a remote entangled state is demonstrated through single-photon-mediated entangling of the electrons and robust storage in the nuclear spins. After applying local two-qubit gates, single-shot measurements herald the distillation of an entangled state with increased fidelity that is available for further use. The key combination of generating, storing, and processing entangled states should enable the exploration of multiparticle entanglement on an extended quantum network.

The realization of a network of quantum registers is an outstanding challenge in quantum science and technology. We experimentally investigate a network node that consists of a single nitrogen-vacancy center electronic spin hyperfine coupled to nearby nuclear spins. We demonstrate individual control and readout of five nuclear spin qubits within one node. We then characterize the storage of quantum superpositions in individual nuclear spins under repeated application of a probabilistic optical internode entangling protocol. We find that the storage fidelity is limited by dephasing during the electronic spin reset after failed attempts. By encoding quantum states into a decoherence-protected subspace of two nuclear spins, we show that quantum coherence can be maintained for over 1000 repetitions of the remote entangling protocol. These results and insights pave the way towards remote entanglement purification and the realization of a quantum repeater using nitrogen-vacancy center quantum-network nodes.

Reliable quantum information processing in the face of errors is a major fundamental and technological challenge. Quantum error correction protects quantum states by encoding a logical quantum bit (qubit) in multiple physical qubits. To be compatible with universal fault-tolerant computations, it is essential that states remain encoded at all times and that errors are actively corrected. Here we demonstrate such active error correction on a continuously protected logical qubit using a diamond quantum processor. We encode the logical qubit in three long-lived nuclear spins, repeatedly detect phase errors by non-destructive measurements, and apply corrections by real-time feedback. The actively error-corrected qubit is robust against errors and encoded quantum superposition states are preserved beyond the natural dephasing time of the best physical qubit in the encoding. These results establish a powerful platform to investigate error correction under different types of noise and mark an important step towards fault-tolerant quantum information processing.