Optically addressable paramagnetic defects in wide-band-gap semiconductors are promising platforms for quantum communications and sensing. The presence of avoided crossings between the electronic levels of these defects can substantially alter their quantum dynamics and be both detrimental and beneficial for quantum information applications. Here we present a joint theoretical and experimental study of the quantum dynamics of paramagnetic defects interacting with a nuclear spin bath at avoided crossings. We find that we can condition the clock transition of the divacancies in SiC on multiple adjacent nuclear spins states. We suppress the effects of fluctuating charge impurities and demonstrate an increased coherence time at clock transition, which is limited purely by magnetic noise. Our results pave the way to designing single defect quantum devices operating at avoided crossings.
Optically addressable paramagnetic defects in wide-band-gap semiconductors are promising platforms for quantum communications and sensing. The presence of avoided crossings between the electronic levels of these defects can substantially alter their quantum dynamics and be both detrimental and beneficial for quantum information applications. Here we present a joint theoretical and experimental study of the quantum dynamics of paramagnetic defects interacting with a nuclear spin bath at avoided crossings. We find that we can condition the clock transition of the divacancies in SiC on multiple adjacent nuclear spins states. We suppress the effects of fluctuating charge impurities and demonstrate an increased coherence time at clock transition, which is limited purely by magnetic noise. Our results pave the way to designing single defect quantum devices operating at avoided crossings.
Divacancy defects in silicon carbide have long-lived electronic spin states and sharp optical transitions. Because of the various polytypes of SiC, hundreds of unique divacancies exist, many with spin properties comparable to the nitrogen-vacancy center in diamond. If ensembles of such spins can be all-optically manipulated, they make compelling candidate systems for quantum-enhanced memory, communication, and sensing applications. We report here direct all-optical addressing of basal plane-oriented divacancy spins in 4H-SiC. By means of magneto-spectroscopy, we fully identify the spin triplet structure of both the ground and the excited state, and use this for tuning of transition dipole moments between particular spin levels. We also identify a role for relaxation via intersystem crossing. Building on these results, we demonstrate coherent population trapping -a key effect for quantum state transfer between spins and photons- for divacancy sub-ensembles along particular crystal axes. These results, combined with the flexibility of SiC polytypes and device processing, put SiC at the forefront of quantum information science in the solid state.
Decoherence limits the physical realization of qubits, and its mitigation is critical for the development of quantum science and technology. We construct a robust qubit embedded in a decoherence-protected subspace, obtained by applying microwave dressing to a clock transition of the ground-state electron spin of a silicon carbide divacancy defect. The qubit is universally protected from magnetic, electric, and temperature fluctuations, which account for nearly all relevant decoherence channels in the solid state. This culminates in an increase of the qubit's inhomogeneous dephasing time by more than four orders of magnitude (to >22 milliseconds), while its Hahn-echo coherence time approaches 64 milliseconds. Requiring few key platform-independent components, this result suggests that substantial coherence improvements can be achieved in a wide selection of quantum architectures.
Abstract Multi-qubit systems are crucial for the advancement and application of quantum science. Such systems require maintaining long coherence times while increasing the number of qubits available for coherent manipulation. For solid-state spin systems, qubit coherence is closely related to fundamental questions of many-body spin dynamics. Here we apply a coherent spectroscopic technique to characterize the dynamics of the composite solid-state spin environment of nitrogen-vacancy colour centres in room temperature diamond. We identify a possible new mechanism in diamond for suppression of electronic spin-bath dynamics in the presence of a nuclear spin bath of sufficient concentration. This suppression enhances the efficacy of dynamical decoupling techniques, resulting in increased coherence times for multi-spin-qubit systems, thus paving the way for applications in quantum information, sensing and metrology.
This thesis describes studies on atomic point defects in semiconductors for applications in quantum information. In particular, its focus is on defects whose energy levels reside deep within the bandgap certain semiconductors because these systems can behave like artificial trapped atoms in the solid state, possessing optical addressability, long coherence times, and the ability to be manipulated at microwave frequencies. The most prominent defect in this field of study is the diamond nitrogen-vacancy center, whose functionality is well-known to persist to ambient temperature. The first part of this thesis investigates the persistence of this functionality to temperatures upwards of 600 K. Importantly, these investigations also demonstrate that the diamond nitrogen-vacancy center can be a sensitive thermometer (~10 mK/Hz^(1/2)) over a wide range of temperatures with nanoscale spatial resolution. The latter part of the thesis describes experimental measurements of divacancy defects in silicon carbide, a potential alternative materials host to diamond with established wafer-scale growth and microfabrication capabilities. Single divacancy spins are isolated and coherently controlled for the first time in the 4H polytype of silicon carbide, and the divacancy's coherence is shown to be a remarkably long T2 = 1.2 ms at T = 20 K. The last chapter extends these results by isolating single divacancies in the 3C polytype, experimentally demonstrating a qualitative and quantitative model of their spin and orbital dynamics, and revealing the divacancy's excited state level structure in both the 3C and 4H polytypes using resonant laser techniques. These excited state transitions are shown to posses a structure identical to the diamond nitrogen-vacancy center and a subset are shown to have favorable cycling properties. The location of a clear spin-photon interface has important implications for high-fidelity quantum state readout and photon-based entanglement schemes that use divacancy spins.
Abstract Virtually noiseless due to the scarcity of spinful nuclei in the lattice, simple oxides hold promise as hosts of solid-state spin qubits. However, no suitable spin defect has yet been found in these systems. Using high-throughput first-principles calculations, we predict spin defects in calcium oxide with electronic properties remarkably similar to those of the NV center in diamond. These defects are charged complexes where a dopant atom — Sb, Bi, or I — occupies the volume vacated by adjacent cation and anion vacancies. The predicted zero phonon line shows that the Bi complex emits in the telecommunication range, and the computed many-body energy levels suggest a viable optical cycle required for qubit initialization. Notably, the high-spin nucleus of each dopant strongly couples to the electron spin, leading to many controllable quantum levels and the emergence of atomic clock-like transitions that are well protected from environmental noise. Specifically, the Hanh-echo coherence time increases beyond seconds at the clock-like transition in the defect with 209Bi. Our results pave the way to designing quantum states with long coherence times in simple oxides, making them attractive platforms for quantum technologies.
Solid-state spin defects are a promising platform for quantum networks. A key requirement is to combine long ground-state spin-coherence times with a coherent optical transition for spin-photon entanglement. Here, we investigate the spin and optical coherence of single nitrogen-vacancy (NV) centres in (111)-grown isotopically engineered diamond. Our diamond-growth process yields a precisely controlled 13C concentration and low-ppb nitrogen concentrations. Combined with the mitigation of 50 Hz noise using a real-time feedforward scheme and tailored decoupling sequences, this enables record defect-electron-spin coherence times of T2=6.8(1) ms for a Hahn echo and of T2DD=11.2(8) s under dynamical decoupling. In addition, we observe coherent optical transitions with a near-lifetime-limited homogeneous linewidth of 16.9(4) MHz and characterize the spectral diffusion dynamics. These results provide new avenues to investigate the incorporation of impurities in diamond and new opportunities for improved spin-qubit control for quantum networks and other quantum technologies.