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Quantum Computing, Communication, and Simulation

Optically detected magnetic resonance in neutral silicon vacancy centers in diamond via bound exciton states

Zi-Huai Zhang, Paul Stevenson, Gergő Thiering, Brendon C. Rose, Ding Huang, Andrew Mark Edmonds, Matthew Markham, S. A. Lyon, Ádám Gali, Nathalie P. de Leon

Published Mar 9, 2022• 0 citations
Publisher

Abstract

Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. In this work, we present the observation of previously unreported optical transitions in SiV0 that are capable of efficiently polarizing the ground state spin. We assign groups of transitions from 825 to 890 nm to higher-lying excited states of SiV0 through a combination of optical and spin measurements. We interpret these spectroscopic lines as transitions to bound exciton states of the defect. Optical spin polarization via these bound exciton states enables the observation of optically detected magnetic resonance of SiV0.

DOI
10.1117/12.2612680

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Neutral silicon vacancy (SiV0) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. In this work, we present the observation of previously unreported optical transitions in SiV0 that are capable of efficiently polarizing the ground state spin. We assign groups of transitions from 825 to 890 nm to higher-lying excited states of SiV0 through a combination of optical and spin measurements. We interpret these spectroscopic lines as transitions to bound exciton states of the defect. Optical spin polarization via these bound exciton states enables the observation of optically detected magnetic resonance of SiV0.
Neutral silicon vacancy (SiV^{0}) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive due to poor understanding of the excited state fine structure and limited off-resonant spin polarization. Here we report the realization of optically detected magnetic resonance and coherent control of SiV^{0} centers at cryogenic temperatures, enabled by efficient optical spin polarization via previously unreported higher-lying excited states. We assign these states as bound exciton states using group theory and density functional theory. These bound exciton states enable new control schemes for SiV^{0} as well as other emerging defect systems.
We demonstrate optical spin polarization of the neutrally charged silicon-vacancy defect in diamond (SiV^{0}), an S=1 defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but nonzero at below-resonant energies. We measure an ensemble spin coherence time T_{2}>100 μs at low-temperature, and a spin relaxation limit of T_{1}>25 s. Optical spin-state initialization around 946 nm allows independent initialization of SiV^{0} and NV^{-} within the same optically addressed volume, and SiV^{0} emits within the telecoms down-conversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that SiV^{0} is a promising candidate for a long-range quantum communication technology.
Neutral silicon-vacancy (Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0) centers in diamond are promising candidates for quantum network applications because of their exceptional optical properties and spin coherence. However, the stabilization of Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers requires careful Fermi-level engineering of the diamond host material, making further technological development challenging. Here, we show that Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers can be efficiently stabilized by photoactivated itinerant carriers. Even in this nonequilibrium configuration, the resulting Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers are stable enough to allow for resonant optical excitation and optically detected magnetic resonance. Our results pave the way for on-demand generation of Si-V0\text{Si-}{V}^{\phantom{\rule{0.1em}{0ex}}0}Si-V0 centers as well as other emerging quantum defects in diamond.
The neutrally charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency optical spin initialization with long spin lifetimes (${T}_{2}\ensuremath{\approx}1$ ms at 4 K) and up to 90% of optical emission into its 946-nm zero-phonon line. However, the electronic structure of SiV0{\mathrm{SiV}}^{0}SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0{\mathrm{SiV}}^{0}SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u^{3}A_{1u}3A1u​ state is incorrect, and identify instead a coupled $^{3}E_{u}\text{\ensuremath{-}}^{3}A_{2u}$ system, the lower state of which has forbidden optical emission at zero stress and efficiently decreases the total emission of the defect. We propose a solution employing finite strain to define a spin-photon interface scheme using SiV0{\mathrm{SiV}}^{0}SiV0 .
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.
We demonstrate the use of two-photon excitation for observing the ground state optically detected magnetic resonance (ODMR) of nitrogen-vacancy centers in diamonds at room temperature. An ultrafast femtosecond laser at 1040 nm was used for excitation, while fluorescence signal read out was achieved through a combination of a PMT and a lock-in amplifier. The imaging capability of two-photon excitation fluorescence (2PEF) was utilized to map the distribution of NV centers in a bulk diamond and micro-sized diamonds. For the first time, ODMR traces of the nitrogen-vacancy center are observed with two-photon excitation, providing a promising tool for fast 3D quantum sensing and imaging.