Nuclear magnetic resonance (NMR) is a powerful method for determining the structure of molecules and proteins [1]. While conventional NMR requires averaging over large ensembles, recent progress with single-spin quantum sensors [2][3][4][5][6][7][8][9] has created the prospect of magnetic imaging of individual molecules [10][11][12][13]. As an initial step towards this goal, isolated nuclear spins and spin pairs have been mapped [14][15][16][17][18][19][20][21]. 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 nuclearnuclear 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 [9][10][11][12][13].The nitrogen-vacancy (NV) centre in diamond has emerged as a powerful quantum sensor [2-13, 22, 23]. The NV electron spin provides long coherence times [5, 6,20] and high-contrast optical readout [5,24,25], enabling high sensitivity over a large range of temperatures [5, 6,20,25,26]. Pioneering experiments with near-surface NV centers have demonstrated spectroscopy of small ensembles of nuclear spins in nano-scale volumes [2, 3,[5][6][7][8], and electron-spin labelled proteins [4]. Furthermore, single nuclear spin sensitivity has been demonstrated and isolated individual nuclear spins and spin pairs have been mapped [14][15][16][17][18][19][20][21]. Together, these results have established the NV center as a promising platform * T.H.Taminiau@TUDelft.nl for magnetic imaging of complex spin systems and single molecules [10][11][12][13].In this work, we realise a key ability towards that goal: the 3D imaging of large nuclear-spin structures with atomic resolution. The main idea of our method is to obtain structural information by accessing the couplings between individual nuclear spins. The key open challenges are: (1) to realize high spectral resolution so that small couplings can be accessed, (2) to isolate such couplings from complex spectra, and (3) to transform the revealed connectivity into the 3D spatial structure with sub-angstrom precision.The basic elements of our experiment are illustrated in Fig. 1a. We consider a cluster of 13 C nuclear spins in the vicinity of a single NV centre in diamond at 4 K. This cluster provides a model system for the magnetic imaging of single molecules and spin ...
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 T Ã 2 ¼ 1.9ð3Þ 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.
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