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Nature Communications

Robust coherent control of solid-state spin qubits using anti-Stokes excitation

Junfeng Wang, Fei-Fei Yan, Qiang Li, Zhenghao Liu, Jin‐Ming Cui, Zhao‐Di Liu, Ádám Gali, Jin‐Shi Xu, Chuan‐Feng Li, Guang‐Can Guo

Published May 28, 2021• 34 citations
Publisher

Abstract

Optically addressable solid-state color center spin qubits have become important platforms for quantum information processing, quantum networks and quantum sensing. The readout of color center spin states with optically detected magnetic resonance (ODMR) technology is traditionally based on Stokes excitation, where the energy of the exciting laser is higher than that of the emission photons. Here, we investigate an unconventional approach using anti-Stokes excitation to detect the ODMR signal of silicon vacancy defect spin in silicon carbide, where the exciting laser has lower energy than the emitted photons. Laser power, microwave power and temperature dependence of the anti-Stokes excited ODMR are systematically studied, in which the behavior of ODMR contrast and linewidth is shown to be similar to that of Stokes excitation. However, the ODMR contrast is several times that of the Stokes excitation. Coherent control of silicon vacancy spin under anti-Stokes excitation is then realized at room temperature. The spin coherence properties are the same as those of Stokes excitation, but with a signal contrast that is around three times greater. To illustrate the enhanced spin readout contrast under anti-Stokes excitation, we also provide a theoretical model. The experiments demonstrate that the current anti-Stokes excitation ODMR approach has promising applications in quantum information processing and quantum sensing.

DOI
10.1038/s41467-021-23471-8

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Optically addressable solid-state color center spin qubits have become important platforms for quantum information processing, quantum networks and quantum sensing. The readout of color center spin states with optically detected magnetic resonance (ODMR) technology is traditionally based on Stokes excitation, where the energy of the exciting laser is higher than that of the emission photons. Here, we investigate an unconventional approach using anti-Stokes excitation to detect the ODMR signal of silicon vacancy defect spin in silicon carbide, where the exciting laser has lower energy than the emitted photons. Laser power, microwave power and temperature dependence of the anti-Stokes excited ODMR are systematically studied, in which the behavior of ODMR contrast and linewidth is shown to be similar to that of Stokes excitation. However, the ODMR contrast is several times that of the Stokes excitation. Coherent control of silicon vacancy spin under anti-Stokes excitation is then realized at room temperature. The spin coherence properties are the same as those of Stokes excitation, but with a signal contrast that is around three times greater. To illustrate the enhanced spin readout contrast under anti-Stokes excitation, we also provide a theoretical model. The experiments demonstrate that the current anti-Stokes excitation ODMR approach has promising applications in quantum information processing and quantum sensing.
The V2 silicon vacancy defect in 4H-SiC has emerged as a promising system for quantum technologies due to its favorable optical and spin properties and the advantages of the SiC host. However, the readout contrast - an important benchmark for quantum sensing - of V2 ensembles for optically-detected magnetic resonance (ODMR) is relatively low, usually <1%\%% at room temperature. To overcome this challenge, we resonantly excite the V2 ensembles at cryogenic temperatures and compare the results with the off-resonant case. We report a maximum ODMR contrast of 50%\%% with only 2 μμμW of resonant laser power, almost 100 times improvement over off-resonant excitation. We attribute this high readout contrast to a subset of V2 centers that have one spin-selective optical transition resonant with the laser. The ODMR contrast decreases with temperature, approaching the non-resonant contrast by 60 K, likely due to broadening of the optical transition linewidths. We achieve a maximum sensitivity of 100 nT/Hz\sqrt{Hz}Hz​ with a resonant laser power of 300 μμμW, while 100 times more non-resonant excitation power is needed to achieve comparable sensitivity.
Color centers in silicon are emerging as promising platforms for quantum technologies. Among them, the G center has attracted considerable interest owing to its bright telecom O-band single-photon emission and its optically addressable metastable electron-spin triplet state. Here we investigate the spin properties of ensembles of G centers under above-band-gap excitation. We elucidate the spin photo-dynamics giving rise to the optical detected magnetic resonance (ODMR) response of G centers. The optimal pulsed sequence for measuring the ODMR spectrum of the G defects is identified, along with the temperature and optical-power regimes maximizing the spin readout contrast. Through magneto-optical measurements, we detect a level-anticrossing of the G center electron spin states. At last, we demonstrate coherent spin control of the defects, and characterize their spin-coherence properties. Unveiling the spin degree of freedom of the G center opens new avenues for the realization of quantum memories and quantum registers based on silicon color centers.
Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light-emitting diodes, and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite anti-Stokes process, where excitation is performed with lower-energy photons. We report that the process is sufficiently efficient to excite even a single quantum system-namely, the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method used to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems and harness it toward the realization of practical nanoscale thermometry and sensing.
Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method employed to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems, and harness it towards the realization of practical nanoscale thermometry and sensing.
Scalable solid-state quantum sensors require simultaneous advances in spin-readout fidelity, photon collection efficiency, and device-level integration, which so far have remained elusive on most material platforms. Here, we overcome these limitations by coupling silicon vacancy spin centers to an array of circular Bragg grating cavities on a scalable thin-film silicon carbide-on-insulator (4H-SiCOI) platform. By employing anti-Stokes excitation, we show that the cavity-enhanced emission compensates for intrinsically weak anti-Stokes absorption, yielding a 24.6-fold increase in collected fluorescence, a high 1.78% spin-readout contrast at zero field, and a 6.42-fold improvement in magnetometry sensitivity. This high spin-readout fidelity further enables the spectroscopic resolution of intrinsic dark-spin bath interactions in 4H-SiCOI, revealing the underlying decoherence mechanisms. Our work establishes cavity-enhanced anti-Stokes excitation as a general and feasible route for silicon carbide quantum technologies, paving the way for scalable manufacturing of spin-based quantum sensors and integrated photonic circuits.
The PL6 color center in silicon carbide has recently emerged as a promising platform for quantum information processing, yet its coherent spin--photon interface has remained largely unexplored. Here we present a comprehensive investigation of single PL6 centers, combining spectroscopy with theoretical analysis. The excited-state fine structure is fully resolved using group-theoretical modeling and strain-dependent measurements. Under resonant excitation, we achieve a spin initialization fidelity of 99.69±0.03%99.69 \pm 0.03\%99.69±0.03% and a readout contrast of 98.31±1.03%98.31 \pm 1.03\%98.31±1.03%. The spin--photon--entangled A2A_2A2​ transition exhibits narrow optical linewidths (∼180\sim 180∼180~MHz) and a polarization visibility of ∼82%\sim 82\%∼82%. Coherent optical driving enables Rabi frequencies up to 2.8952.8952.895~GHz, while dynamical decoupling extends the spin coherence time from 0.50.50.5~ms to 5.705.705.70~ms. Our results establish PL6 as a competitive solid-state spin--photon interface hosted in a commercially available semiconductor platform.