Solid-state spin qubits is a promising platform for quantum computation and quantum networks1,2. Recent experiments have demonstrated high-quality control over multi-qubit systems3–8, elementary quantum algorithms8–11 and non-fault-tolerant error correction12–14. Large-scale systems will require using error-corrected logical qubits that are operated fault tolerantly, so that reliable computation becomes possible despite noisy operations15–18. Overcoming imperfections in this way remains an important outstanding challenge for quantum science15,19–27. 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 qubits28–30. 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.@en

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.@en

Entanglement distribution over quantum networks has the promise of realizing fundamentally new technologies. Entanglement between separated quantum processing nodes has been achieved on several experimental platforms in the past decade. To move toward metropolitan-scale quantum network test beds, the creation and transmission of indistinguishable single photons over existing telecom infrastructure is key. Here, we report the interference of photons emitted by remote spectrally detuned NV-center-based network nodes, using quantum frequency conversion to the telecom L band. We find a visibility of 0.79±0.03 and an indistinguishability between converted NV photons around 0.9 over the full range of the emission duration, confirming the removal of the spectral information present. Our approach implements fully separated and independent control over the nodes, time multiplexing of control and quantum signals, and active feedback to stabilize the output frequency. Our results demonstrate a working principle that can be readily employed on other platforms and shows a clear path toward generating metropolitan-scale solid-state entanglement over deployed telecom fibers.@en

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.@en

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. @en

The neutral charge state plays an important role in quantum information and sensing applications basedon nitrogen-vacancy centers. However, the orbital and spin dynamics remain unexplored. Here, we useresonant excitation of single centers to directly reveal the fine structure, enabling selective addressing ofspin-orbit states. Through pump-probe experiments, we find the orbital relaxation time (430 ns at 4.7 K)and measure its temperature dependence up to 11.8 K. Finally, we reveal the spin relaxation time (1.5 s) andrealize projective high-fidelity single-shot readout of the spin state (≥98%).@en

Electron spin qubits associated with individual solid-state defects can exhibit exceptional coherence and bright optical interfaces. Furthermore, their magnetic interactions with nuclear spins in the host material present a resource for multi-qubit registers. They have thus emerged as powerful systems with which to develop quantum technologies. In this thesis, we develop a toolbox for the precise control of multi-qubit spin systems associated with single nitrogen-vacancy centres in diamond. We utilise this platform to explore a number of avenues in quantum science: networks, computation, sensing, and simulation. Our findings provide new insights towards the goal of distributed quantum computation, and establish a programmable solid-state-spin quantum simulator for studying many-body physics.@en

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.@en

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.@en

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.@en

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.@en

We demonstrate interference of photons emitted by remote, spectrally distinct NV-centers. Quantum frequency conversion at the nodes brings the photons to the same wavelength in the telecom L-band, compatible with entanglement generation at metropolitan scale.@en

We demonstrate interference of photons emitted by remote, spectrally distinct NV-centers. Quantum frequency conversion at the nodes brings the photons to the same wavelength in the telecom L-band, compatible with entanglement generation at metropolitan scale.@en

We demonstrate interference of photons emitted by remote, spectrally distinct NV-centers. Quantum frequency conversion at the nodes brings the photons to the same wavelength in the telecom L-band, compatible with entanglement generation at metropolitan scale.@en

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 sensors2–9 has created the prospect of magnetic imaging of individual molecules10–13. As an initial step towards this goal, isolated nuclear spins and spin pairs have been mapped14–21. 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 systems9–13.@en