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    High-resolution nanoscale NMR for arbitrary magnetic fields
    (2023) Meinel, Jonas; Kwon, MinSik; Maier, Rouven; Dasari, Durga; Sumiya, Hitoshi; Onoda, Shinobu; Isoya, Junichi; Vorobyov, Vadim; Wrachtrup, Jörg
    Nitrogen vacancy (NV) centers are a major platform for the detection of nuclear magnetic resonance (NMR) signals at the nanoscale. To overcome the intrinsic electron spin lifetime limit in spectral resolution, a heterodyne detection approach is widely used. However, application of this technique at high magnetic fields is yet an unsolved problem. Here, we introduce a heterodyne detection method utilizing a series of phase coherent electron nuclear double resonance sensing blocks, thus eliminating the numerous Rabi microwave pulses required in the detection. Our detection protocol can be extended to high magnetic fields, allowing chemical shift resolution in NMR experiments. We demonstrate this principle on a weakly coupled 13 C nuclear spin in the bath surrounding single NV centers, and compare the results to existing heterodyne protocols. Additionally, we identify the combination of NV-spin-initialization infidelity and strong sensor-target-coupling as linewidth-limiting decoherence source, paving the way towards high-field heterodyne NMR protocols with chemical resolution.
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    Reducing inhomogeneous broadening of spin and optical transitions of nitrogen-vacancy centers in high-pressure, high-temperature diamond
    (2024) Blinder, Rémi; Mindarava, Yuliya; Tran, Thai Hien; Momenzadeh, Ali; Yang, Sen; Siyushev, Petr; Sumiya, Hitoshi; Tamasaku, Kenji; Osaka, Taito; Morishita, Norio; Takizawa, Haruki; Onoda, Shinobu; Hara, Hideyuki; Jelezko, Fedor; Wrachtrup, Jörg; Isoya, Junichi
    With their optical addressability of individual spins and long coherence time, nitrogen-vacancy (NV) centers in diamond are often called “atom-like solid spin-defects”. As observed with trapped atomic ions, quantum interference mediated by indistinguishable photons was demonstrated between remote NV centers. In high sensitivity DC magnetometry at room temperature, NV ensembles are potentially rivaling with alkali-atom vapor cells. However, local strain induces center-to-center variation of both optical and spin transitions of NV centers. Therefore, advanced engineering of diamond growth toward crystalline perfection is demanded. Here, we report on the synthesis of high-quality HPHT (high-pressure, high-temperature) crystals, demonstrating a small inhomogeneous broadening of the spin transitions, of T2* = 1.28 μs, approaching the limit for crystals with natural 13C abundance, that we determine as T2* = 1.48 μs. The contribution from strain and local charges to the inhomogeneous broadening is lowered to ~17 kHz full width at half maximum for NV ensemble within a > 10 mm3 volume. Looking at optical transitions in low nitrogen crystals, we examine the variation of zero-phonon-line optical transition frequencies at low temperatures, showing a strain contribution below 2 GHz for a large fraction of single NV centers.