Magnetocardiography is a contactless imaging modality for electric current propagation in the cardiovascular system. Although conventional sensors provide sufficiently high sensitivity, their spatial resolution is limited to a centimetre-scale, which is inadequate for revealing the intra-cardiac electrodynamics such as rotational waves associated with ventricular arrhythmias. Here, we demonstrate invasive magnetocardiography of living rats at a millimetre-scale using a quantum sensor based on nitrogen-vacancy centres in diamond. The acquired magnetic images indicate that the cardiac signal source is well explained by vertically distributed current dipoles, pointing from the right atrium base via the Purkinje fibre bundle to the left ventricular apex. We also find that this observation is consistent with and complementary to an alternative picture of electric current density distribution calculated with a stream function method. Our technique will enable the study of the origin and progression of various cardiac arrhythmias, including flutter, fibrillation, and tachycardia.
We investigated spin-echo coherence times T2 of negatively charged nitrogen vacancy center (NV−) ensembles in single-crystalline diamond synthesized by either the high-pressure and high-temperature and chemical vapor deposition methods. This study specifically examined the magnetic dipole–dipole interaction (DDI) from the various electronic spin baths, which are the source of T2 decoherence. Diamond samples with NV− center concentration [NV−] comparable to those of neutral substitutional nitrogen concentration [Ns0] were used for DDI estimation. Results show that the T2 of the ensemble NV− center decreased in inverse proportion to the concentration of nitrogen-related paramagnetic defects [NPM], being the sum of [Ns0], [NV−], and [NV0], which is a neutrally charged state NV center. This inversely proportional relation between T2 and [NPM] indicates that the nitrogen-related paramagnetic defects of three kinds are the main decoherence source of the ensemble NV− center in the single-crystalline diamond. We found that the DDI coefficient of NVH− center was significantly smaller than that of Ns0, the NV0 center, or the NV− center. We ascertained the DDI coefficient of the NV− center [Formula: see text] through experimentation using a linear summation of the decoherence rates of each nitrogen-related paramagnetic defect. The obtained value of 89 μs ppm for [Formula: see text] corresponds well to the value estimated from the relation between DDI coefficient and spin multiplicity.
Controllability of nitrogen doping, types of nitrogen-related defects, and their charge states in homoepitaxial diamond (001) crystals were investigated. For these purposes, 15N-doped 12C-enriched free-standing chemical vapor deposited diamond (001) crystals were grown through long-time growth using 12C-enriched methane as the carbon source gas and 15N-enriched molecular nitrogen as the nitrogen source gas. The formation of non-epitaxial crystallites and growth hillocks was suppressed by the application of the oxygen-adding growth condition. Nitrogen was incorporated uniformly into the crystals, with a concentration variation of less than 10%. About 70% of the total nitrogen was substitutional nitrogen in a neutral charge state Ns0. Hydrogen was incorporated at approximately the same concentration as nitrogen. Both NV and NVH centers were predominantly negatively charged defect structures, i.e., NV− and NHV− centers. The concentrations of NHV− centers were less than 5% of the total nitrogen concentration. Nitrogen concentration in diamond crystals was controlled by changing the N/C gas ratio over a wide doping range from 10 ppb to 10 ppm. Nitrogen incorporation efficiency was found to be (1.5 ± 0.5) × 10−4 in this study.
We investigated charge states of nitrogen vacancy (NV) centers in diamond single crystals. The charge states were evaluated using concentrations of both negatively charged (NV−) and neutral-state (NV0) NV centers. This study specifically examines diamond crystals containing mainly neutral substitutional nitrogen (N0s), NV− centers, and NV0 centers. Results show that the charged states of NV centers evaluated for this study depended on concentrations of both neutral substitutional nitrogen (N0s) and NVT centers, which is a sum of [NV−] and [NV0]. The NV centers were fully negatively charged when the ratio of [NVT] to [N0s] was 1%–20% in our diamond crystals. When [NVT]/[N0s] is larger than 20%–30%, NV0 centers appeared gradually. The concentration ratio between NV− centers and NV0 centers was described using an equilibrium equation.
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