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arXiv:1802.06714 · npj Quantum Information

Identification and tunable optical coherent control of transition-metal spins in silicon carbide

Tom Bosma, Gerrit J. J. Lof, Carmem M. Gilardoni, Olger V. Zwier, Freddie Hendriks, Björn Magnusson, Alexandre Ellison, Andreas Gällström, Ivan Gueorguiev Ivanov, N. T. Son, Remco W. A. Havenith, Caspar H. van der Wal

Published Sep 25, 2018• 70 citations
arXivHTMLPDF

Abstract

Abstract Color centers in wide-bandgap semiconductors are attractive systems for quantum technologies since they can combine long-coherent electronic spin and bright optical properties. Several suitable centers have been identified, most famously the nitrogen-vacancy defect in diamond. However, integration in communication technology is hindered by the fact that their optical transitions lie outside telecom wavelength bands. Several transition-metal impurities in silicon carbide do emit at and near telecom wavelengths, but knowledge about their spin and optical properties is incomplete. We present all-optical identification and coherent control of molybdenum-impurity spins in silicon carbide with transitions at near-infrared wavelengths. Our results identify spin S = 1/2 for both the electronic ground and excited state, with highly anisotropic spin properties that we apply for implementing optical control of ground-state spin coherence. Our results show optical lifetimes of ~60 ns and inhomogeneous spin dephasing times of ~0.3 μs, establishing relevance for quantum spin-photon interfacing.

DOI
10.1038/s41534-018-0097-8

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Abstract Color centers in wide-bandgap semiconductors are attractive systems for quantum technologies since they can combine long-coherent electronic spin and bright optical properties. Several suitable centers have been identified, most famously the nitrogen-vacancy defect in diamond. However, integration in communication technology is hindered by the fact that their optical transitions lie outside telecom wavelength bands. Several transition-metal impurities in silicon carbide do emit at and near telecom wavelengths, but knowledge about their spin and optical properties is incomplete. We present all-optical identification and coherent control of molybdenum-impurity spins in silicon carbide with transitions at near-infrared wavelengths. Our results identify spin S = 1/2 for both the electronic ground and excited state, with highly anisotropic spin properties that we apply for implementing optical control of ground-state spin coherence. Our results show optical lifetimes of ~60 ns and inhomogeneous spin dephasing times of ~0.3 μs, establishing relevance for quantum spin-photon interfacing.
Solid-state color centers with manipulatable spin qubits and telecom-ranged fluorescence are ideal platforms for quantum communications and distributed quantum computations. In this work, we coherently control the nitrogen-vacancy (NV) center spins in silicon carbide at room temperature, in which telecom-wavelength emission is detected. We increase the NV concentration sixfold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature, and the coherence time T_{2} can be reached to around 17.1 μs. Furthermore, an investigation of fluorescence properties of single NV centers shows that they are room-temperature photostable single-photon sources at telecom range. Taking advantage of technologically mature materials, the experiment demonstrates that the NV centers in silicon carbide are promising platforms for large-scale integrated quantum photonics and long-distance quantum networks.
Abstract Spin impurities in diamond have emerged as a promising building block in a wide range of solid-state-based quantum technologies. The negatively charged silicon-vacancy centre combines the advantages of its high-quality photonic properties with a ground-state electronic spin, which can be read out optically. However, for this spin to be operational as a quantum bit, full quantum control is essential. Here we report the measurement of optically detected magnetic resonance and the demonstration of coherent control of a single silicon-vacancy centre spin with a microwave field. Using Ramsey interferometry, we directly measure a spin coherence time, T2*, of 115±9 ns at 3.6 K. The temperature dependence of coherence times indicates that dephasing and decay of the spin arise from single-phonon-mediated excitation between orbital branches of the ground state. Our results enable the silicon-vacancy centre spin to become a controllable resource to establish spin-photon quantum interfaces.
Color centers in wide bandgap semiconductors are prominent candidates for solid-state quantum technologies due to their attractive properties including optical interfacing, long coherence times, and spin–photon and spin–spin entanglement, as well as the potential for scalability. Silicon carbide color centers integrated into photonic devices span a wide range of applications in quantum information processing in a material platform with quantum-grade wafer availability and advanced processing capabilities. Recent progress in emitter generation and characterization, nanofabrication, device design, and quantum optical studies has amplified the scientific interest in this platform. We provide a conceptual and quantitative analysis of the role of silicon carbide integrated photonics in three key application areas: quantum networking, simulation, and computing.
Quantum networks require qubits that combine efficient optical access, coherent control, and long-lived quantum memory, but realizing all three in one scalable platform remains a central bottleneck. Diamond color centers are leading candidates, yet widely studied defects retain tradeoffs among these capabilities. Here, we show that transition-metal defects in diamond provide a distinct route beyond these platforms by combining spin-orbit protected ground-state coherence, all-optical control, and near-infrared emission. Using a single nickel-vacancy (NiV−^-−), we demonstrate an all-optically controlled diamond spin qubit with coherence exceeding one millisecond at 1.65 K, compatible with compact closed-cycle cryogenics. We implement Raman Rabi oscillations and Ramsey interferometry and use all-optical dynamical decoupling to extend coherence from T2∗T_2^*T2∗​ = 371 ns to T2CPMG−4T_2^{CPMG-4}T2CPMG−4​ = 1.27 ms, establishing NiV−^-− as a deployable diamond spin-photon interface.
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.
Spin impurities in diamond can be versatile tools for a wide range of solid-state-based quantum technologies, but finding spin impurities that offer sufficient quality in both photonic and spin properties remains a challenge for this pursuit. The silicon-vacancy center has recently attracted much interest because of its spin-accessible optical transitions and the quality of its optical spectrum. Complementing these properties, spin coherence is essential for the suitability of this center as a spin-photon quantum interface. Here, we report all-optical generation of coherent superpositions of spin states in the ground state of a negatively charged silicon-vacancy center using coherent population trapping. Our measurements reveal a characteristic spin coherence time, T2*, exceeding 45 nanoseconds at 4 K. We further investigate the role of phonon-mediated coupling between orbital states as a source of irreversible decoherence. Our results indicate the feasibility of all-optical coherent control of silicon-vacancy spins using ultrafast laser pulses.