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arXiv:1905.06405 · Physical Review Letters

Extending the Quantum Coherence of a Near-Surface Qubit by Coherently Driving the Paramagnetic Surface Environment

Dolev Bluvstein, Zhiran Zhang, Claire A. McLellan, Nicolas R. Williams, Ania C. Bleszynski Jayich

Published Oct 4, 2019• 40 citations
arXivHTMLPDF

Abstract

Surfaces enable useful functionalities for quantum systems, e.g., as interfaces to sensing targets, but often result in surface-induced decoherence where unpaired electron spins are common culprits. Here we show that the coherence time of a near-surface qubit is increased by coherent radio-frequency driving of surface electron spins, where we use a diamond nitrogen-vacancy (NV) center as a model qubit. This technique is complementary to other methods of suppressing decoherence and, importantly, requires no additional materials processing or control of the qubit. Further, by combining driving with the increased magnetic susceptibility of the double-quantum basis, we realize an overall fivefold sensitivity enhancement in NV magnetometry. Informed by our results, we discuss a path toward relaxation-limited coherence times for near-surface NV centers. The surface-spin driving technique presented here is broadly applicable to a wide variety of qubit platforms afflicted by surface-induced decoherence.

DOI
10.1103/physrevlett.123.146804

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Surfaces enable useful functionalities for quantum systems, e.g., as interfaces to sensing targets, but often result in surface-induced decoherence where unpaired electron spins are common culprits. Here we show that the coherence time of a near-surface qubit is increased by coherent radio-frequency driving of surface electron spins, where we use a diamond nitrogen-vacancy (NV) center as a model qubit. This technique is complementary to other methods of suppressing decoherence and, importantly, requires no additional materials processing or control of the qubit. Further, by combining driving with the increased magnetic susceptibility of the double-quantum basis, we realize an overall fivefold sensitivity enhancement in NV magnetometry. Informed by our results, we discuss a path toward relaxation-limited coherence times for near-surface NV centers. The surface-spin driving technique presented here is broadly applicable to a wide variety of qubit platforms afflicted by surface-induced decoherence.
We probe the relaxation dynamics of the full three-level spin system of near-surface nitrogen-vacancy (NV) centers in diamond to define a T_{1} relaxation time that sets the T_{2}≤2T_{1} coherence limit of the NV's subset qubit superpositions. We find that double-quantum spin relaxation via electric field noise dominates T_{1} of near-surface NVs at low applied magnetic fields. Furthermore, we differentiate 1/f^{α} spectra of electric and magnetic field noise using a novel noise-spectroscopy technique, with broad applications in probing surface-induced decoherence at material interfaces.
Nitrogen vacancy centers (NV) in proximity to diamond surfaces are promising nanoscale quantum sensors. However, their coherence properties are negatively affected by magnetic and electric surface noise, whose origin and detailed impact have remained elusive. Using atomistic models of diamond surfaces derived with density functional theory, together with decoherence time calculations with cluster correlation expansion methods, we quantify the effects of surface crystallographic orientation and functionalization, and of the density of unpaired electrons on the NV Hahn-echo time T2T_2T2​. We determine a crossover depth at which T2T_2T2​ ceases to be limited by surface nuclear spins and recovers the bulk-limited value. We find that for static surface-electron baths, the ratio between the NV depth and the separation between surface electron spins determines a transition from fast-fluctuating to quasi-static noise, leading to a dependence of T2T_2T2​ on orientation for specific surfaces. We also find that the modulation of T2T_2T2​ by spin-phonon relaxations leads to motional-narrowing at sub-microsecond relaxation times. Importantly, our calculations show that it is only when accounting for surface-spin in-sequence hopping that measured T2T_2T2​ values as a function of depth can be reproduced, thus highlighting the importance of hopping-mediated models to describe the surface spin noise affecting NV sensors. Overall, our work provides clear guidelines for engineering diamond surfaces to achieve enhanced NV coherence for quantum sensing and information processing applications.
Nitrogen-vacancy (NV) centers in diamond are utilized extensively as quantum sensors for imaging fields at the nanoscale. The ultrahigh sensitivity of NV magnetometers has enabled the detection and spectroscopy of individual electron spins, with potentially far-reaching applications in condensed matter physics, spintronics, and molecular biology. However, the surfaces of these diamond sensors naturally contain electron spins, which create a background signal that can be hard to differentiate from the signal of the target spins. In this study, we develop a surface modification approach that eliminates the unwanted signal of these so-called dark electron spins. Our surface passivation technique, based on coating diamond surfaces with a thin titanium oxide ( Ti O 2 ) layer, reduces the dark spin density. The observed reduction in dark spin density aligns with our findings on the electronic structure of the diamond- Ti O 2 interface. The reduction, from a typical value of 2000 μ m − 2 to a value below that set by the detection limit of our NV sensors ( 200 μ m − 2 ), results in a twofold increase in Hahn-echo coherence time of near surface NV centers. Furthermore, we derive a comprehensive spin model that connects dark spin relaxation with NV coherence, providing additional insights into the mechanisms behind the observed spin dynamics. Our findings are directly transferable to other quantum platforms, including nanoscale solid-state qubits and superconducting qubits.
High spatial resolution quantum sensing of near-surface nitrogen vacancy (NV) centers in diamond has enabled detection of magnetic, electrical, and thermal signals at the nanoscale. At depths of just a few nanometers, NV centers serve as localized quantum probes for external spins or low-dimensional materials, but their proximity to the surface also enhances decoherence caused by fluctuating nuclear spins. While advances in surface engineering have stabilized the charge state of NV centers at depths of tens of nanometers, achieving both ultra-shallow implantation (0.5-2 nm) and long-term spin coherence remains a central challenge. In this work, we show using first-principles modeling that, by exploiting the interaction of surface-induced strain and weak dc magnetic fields, the spin coherence times of 1-nm-deep NV centers can be greatly improved near the spin-phonon-confined regime at room temperature in 12C-rich diamonds. We also demonstrate that this protocol benefits ~ 10-nm-deep NV centers in natural diamond, enabling vector magnetometry at the nanoscale. Shallow NV centers in diamond are advantageous for quantum sensing but suffer from surface magnetic noise. Using first-principles simulations supported by experiments, the authors show that a combination of small magnetic fields and surface strain can significantly enhance spin coherence of 1 nm-deep NV centers.
Nanoscale quantum probes such as the nitrogen-vacancy (NV) center in diamonds have demonstrated remarkable sensing capabilities over the past decade as control over fabrication and manipulation of these systems has evolved. The biocompatibility and rich surface chemistry of diamonds has added to the utility of these probes but, as the size of these nanoscale systems is reduced, the surface chemistry of diamond begins to impact the quantum properties of the NV center. In this work, we systematically study the effect of the diamond surface chemistry on the quantum coherence of the NV center in nanodiamonds (NDs) 50 nm in size. Our results show that a borane-reduced diamond surface can on average double the spin relaxation time of individual NV centers in nanodiamonds when compared to thermally oxidized surfaces. Using a combination of infrared and X-ray absorption spectroscopy techniques, we correlate the changes in quantum relaxation rates with the conversion of sp 2 carbon to C–O and C–H bonds on the diamond surface. These findings implicate double-bonded carbon species as a dominant source of spin noise for near surface NV centers. The link between the surface chemistry and quantum coherence indicates that through tailored engineering of the surface, the quantum properties and magnetic sensitivity of these nanoscale systems may approach that observed in bulk diamond.
Quantum coherence serves as a crucial quantum resource for achieving high-sensitivity quantum sensing. Because of its long coherence time at room temperature, the nitrogen-vacancy (NV) center has emerged as a quantum sensor in various fields in recent years. While nanoscale quantum sensing at room temperature has been demonstrated for NV centers, noise on the diamond surface severely limits its further development at a higher sensitivity. Here, we utilize the hybridization between graphene and diamond surfaces to directly deplete surface unpaired electron spins, thereby achieving roughly two-fold enhancement in coherence. Through the combination of electron spin resonance spectra and first-principle calculations, we explain that this phenomenon arises from a significant reduction in electron spin density on the diamond surface due to interface electron orbital hybridization. Our research presents a new approach for solid-state quantum sensors to reach the desired sensitivity level and offers a new pathway for future studies on material interfaces.