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Bulletin of the American Physical Society

Quantum Synchronization in Nitrogen-Vacancy Centers in Diamonds

Pronoy Das, Agam Verma, Parvinder Solanki, Abhishek Kejriwal, Shreyas Chandgothia, Sai Vinjanampathy, Kasturi Saha

Published Mar 16, 2021• 0 citations
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Nitrogen vacancy centers in diamond (NVs) are point defects well suited to quantum sensing of magnetic fields. NV spin states can be initialized and read out optically with high spatial resolution, enabling detection of pL-scale volumes of nuclear spins. Using Coherently Averaged Synchronized Readout (CASR), standard NMR spectroscopy techniques such as free decay, spin echo, and PGSE have been performed with Hz-scale spectral resolution using NV-diamond sensors. However, using NV detection for conventional high-resolution NMR at multi-tesla fields is challenging due to the need to manipulate NV electronic spins at resonance frequencies 100 GHz or higher. Low-field J-coupling spectroscopy provides an alternative path to chemical resolution in a regime more easily accessible to NVs. Here, we demonstrate homonuclear and heteronuclear J-coupling spectroscopy using an NV-NMR spectrometer based on permanent magnets operating at $\sim$890 kHz proton Larmor frequency (bias magnetic field $\sim$21 mT). This field strength enables chemical characterization based on J-coupling using sequences such as Synchronized Echo (SyncE) and Spin-Echo Double Resonance (SEDOR), which do not require the strong chemical shift dispersion and pristine field homogeneity of high-field NMR. The frequency range is easily detected by NVs using standard XY dynamical decoupling sequences and is well-suited for applying Overhauser DNP, which can boost proton signal by two orders of magnitude. We acquire initial NV-NMR measurements of T$_1$, T$_2$, and Overhauser DNP in glycerol before advancing to SEDOR spectroscopy of methanol-$^{13}$C and a methanol-$^{13}$C/acetonitrile-2-$^{13}$C mixture at sample volumes $\sim$50 pL, in which we demonstrate measurement of $^1J_\text{CH}$ couplings and resolution between species. We also acquire a homonuclear J-coupling spectrum of a natural-abundance propylene carbonate sample.

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Effect of fluorinated diamond surface on charge state of nitrogen-vacancy centers

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Abstract The nitrogen-vacancy (NV) center in diamond is the most promising candidate for quantum sensing because of its beneficial properties. For quantum-sensing applications, a shallow NV center is critical for approximating the sensing target on a diamond surface. Such shallow NV centers are strongly affected by the diamond surface termination. The properties of shallow NV centers in hydrogen-, oxygen-, and fluorine-terminated diamond have been well studied. In recent years, silicon-terminated diamond has also been investigated; however, the effect of silicon-terminated diamond on the properties of shallow NV centers remains unclear. Recently, the suitability of nitrogen-terminated diamond for shallow NV centers has been theoretically and experimentally examined; however, quantum sensing has not yet been performed. In this work, we evaluated the effect of silicon and nitrogen termination on shallow NV centers. The negatively charged state of shallow NV centers was unstable below silicon termination. In contrast, the properties of shallow NV centers in nitrogen-terminated diamond were satisfactory for quantum sensing and enabled 1H NMR detection. Our results are in good agreement with previous reports on silicon and nitrogen terminations and provide the perspective that the stability of shallow NV centers highly depends on the polarity of electron affinity of the diamond surface.

The Journal of Physical Chemistry C•Jan 24, 2019•93 citations
Nitrogen vacancy centers in diamond (NVs) are point defects well suited to quantum sensing of magnetic fields. NV spin states can be initialized and read out optically with high spatial resolution, enabling detection of pL-scale volumes of nuclear spins. Using Coherently Averaged Synchronized Readout (CASR), standard NMR spectroscopy techniques such as free decay, spin echo, and PGSE have been performed with Hz-scale spectral resolution using NV-diamond sensors. However, using NV detection for conventional high-resolution NMR at multi-tesla fields is challenging due to the need to manipulate NV electronic spins at resonance frequencies 100 GHz or higher. Low-field J-coupling spectroscopy provides an alternative path to chemical resolution in a regime more easily accessible to NVs. Here, we demonstrate homonuclear and heteronuclear J-coupling spectroscopy using an NV-NMR spectrometer based on permanent magnets operating at $\sim$890 kHz proton Larmor frequency (bias magnetic field $\sim21mT).ThisfieldstrengthenableschemicalcharacterizationbasedonJ−couplingusingsequencessuchasSynchronizedEcho(SyncE)andSpin−EchoDoubleResonance(SEDOR),whichdonotrequirethestrongchemicalshiftdispersionandpristinefieldhomogeneityofhigh−fieldNMR.ThefrequencyrangeiseasilydetectedbyNVsusingstandardXYdynamicaldecouplingsequencesandiswell−suitedforapplyingOverhauserDNP,whichcanboostprotonsignalbytwoordersofmagnitude.WeacquireinitialNV−NMRmeasurementsofT21 mT). This field strength enables chemical characterization based on J-coupling using sequences such as Synchronized Echo (SyncE) and Spin-Echo Double Resonance (SEDOR), which do not require the strong chemical shift dispersion and pristine field homogeneity of high-field NMR. The frequency range is easily detected by NVs using standard XY dynamical decoupling sequences and is well-suited for applying Overhauser DNP, which can boost proton signal by two orders of magnitude. We acquire initial NV-NMR measurements of T21mT).ThisfieldstrengthenableschemicalcharacterizationbasedonJ−couplingusingsequencessuchasSynchronizedEcho(SyncE)andSpin−EchoDoubleResonance(SEDOR),whichdonotrequirethestrongchemicalshiftdispersionandpristinefieldhomogeneityofhigh−fieldNMR.ThefrequencyrangeiseasilydetectedbyNVsusingstandardXYdynamicaldecouplingsequencesandiswell−suitedforapplyingOverhauserDNP,whichcanboostprotonsignalbytwoordersofmagnitude.WeacquireinitialNV−NMRmeasurementsofT_1,T, T,T_2,andOverhauserDNPinglycerolbeforeadvancingtoSEDORspectroscopyofmethanol−, and Overhauser DNP in glycerol before advancing to SEDOR spectroscopy of methanol-,andOverhauserDNPinglycerolbeforeadvancingtoSEDORspectroscopyofmethanol−^{13}Candamethanol−C and a methanol-Candamethanol−^{13}C/acetonitrile−2−C/acetonitrile-2-C/acetonitrile−2−^{13}$C mixture at sample volumes $\sim$50 pL, in which we demonstrate measurement of 1JCH^1J_\text{CH}1JCH​ couplings and resolution between species. We also acquire a homonuclear J-coupling spectrum of a natural-abundance propylene carbonate sample.
We investigated the effect of fluorine-terminated diamond surface on the charged state of shallow nitrogen vacancy defect centers (NVs). Fluorination is achieved with CF4 plasma and the surface chemistry is confirmed with x-ray photoemission spectroscopy. Photoluminescence of these ensemble NVs reveal that fluorine-treated surfaces lead to a higher negatively charged nitrogen vacancy (NV-) population than oxygen-terminated surfaces. Using surface chemistry to control NV charges, in particular increasing the density of NV- centers, is an important step towards improving the optical and spin properties of NVs for quantum information processing and magnetic sensing.
Abstract The nitrogen-vacancy (NV) center in diamond is the most promising candidate for quantum sensing because of its beneficial properties. For quantum-sensing applications, a shallow NV center is critical for approximating the sensing target on a diamond surface. Such shallow NV centers are strongly affected by the diamond surface termination. The properties of shallow NV centers in hydrogen-, oxygen-, and fluorine-terminated diamond have been well studied. In recent years, silicon-terminated diamond has also been investigated; however, the effect of silicon-terminated diamond on the properties of shallow NV centers remains unclear. Recently, the suitability of nitrogen-terminated diamond for shallow NV centers has been theoretically and experimentally examined; however, quantum sensing has not yet been performed. In this work, we evaluated the effect of silicon and nitrogen termination on shallow NV centers. The negatively charged state of shallow NV centers was unstable below silicon termination. In contrast, the properties of shallow NV centers in nitrogen-terminated diamond were satisfactory for quantum sensing and enabled 1H NMR detection. Our results are in good agreement with previous reports on silicon and nitrogen terminations and provide the perspective that the stability of shallow NV centers highly depends on the polarity of electron affinity of the diamond surface.