Quantum networks can enable quantum communication and modular quantum computation. A powerful approach is to use multi-qubit nodes that provide quantum memory and computational power. Nuclear spins associated with defects in diamond are promising qubits for this role. However, dephasing during optical entanglement distribution hinders scaling to larger systems. Here, we show that a ¹³C-spin quantum memory in isotopically engineered diamond is robust to the optical link operation of a nitrogen-vacancy centre. The memory lifetime is improved by two orders-of-magnitude upon the state-of-the-art, surpassing reported times for entanglement distribution. Additionally, we demonstrate that the nuclear-spin state can survive ionisation and recapture of the nitrogen-vacancy electron. Finally, we use simulations to show that combining this memory with previously demonstrated entanglement links and gates can enable key network primitives, such as deterministic non-local two-qubit gates, paving the way for test-bed quantum networks capable of investigating complex algorithms and error correction.

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.

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.

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 N14 atoms. In contrast, NV centers formed from implanted N15 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.