The key challenge in experimental quantum information science is to identify isolated quantum mechanical systems with long coherence times that can be manipulated and coupled together in a scalable fashion. We describe the coherent manipulation of an individual electron spin and nearby individual nuclear spins to create a controllable quantum register. Using optical and microwave radiation to control an electron spin associated with the nitrogen vacancy (NV) color center in diamond, we demonstrated robust initialization of electron and nuclear spin quantum bits (qubits) and transfer of arbitrary quantum states between them at room temperature. Moreover, nuclear spin qubits could be well isolated from the electron spin, even during optical polarization and measurement of the electronic state. Finally, coherent interactions between individual nuclear spin qubits were observed and their excellent coherence properties were demonstrated. These registers can be used as a basis for scalable, optically coupled quantum information systems.

Quantum entanglement is among the most fascinating aspects of quantum theory¹. Entangled optical photons are now widely used for fundamental tests of quantum mechanics² and applications such as quantum cryptography¹. Several recent experiments demonstrated entanglement of optical photons with trapped ions³, atoms^4,5 and atomic ensembles^6,7,8, which are then used to connect remote long-term memory nodes in distributed quantum networks^9,10,11. Here we realize quantum entanglement between the polarization of a single optical photon and a solid-state qubit associated with the single electronic spin of a nitrogen vacancy centre in diamond. Our experimental entanglement verification uses the quantum eraser technique^5,12, and demonstrates that a high degree of control over interactions between a solid-state qubit and the quantum light field can be achieved. The reported entanglement source can be used in studies of fundamental quantum phenomena and provides a key building block for the solid-state realization of quantum optical networks^13,14.

The negatively charged silicon vacancy (SiV) color center in diamond has recently proven its suitability for bright and stable single photon emission. However, its electronic structure so far has remained elusive. We here explore the electronic structure by exposing single SiV defects to a magnetic field where the Zeeman effect lifts the degeneracy of magnetic sublevels. The similar responses of single centers and a SiV ensemble in a low strain reference sample prove our ability to fabricate almost perfect single SiVs, revealing the true nature of the defect's electronic properties. We model the electronic states using a group-theoretical approach yielding a good agreement with the experimental observations. Furthermore, the model correctly predicts polarization measurements on single SiV centers and explains recently discovered spin selective excitation of SiV defects.