Magnetometers based on nitrogen-vacancy (NV) centers in diamond are promising room-temperature, solidstate sensors. However, their reported sensitivity to magnetic fields at low frequencies (1 kHz) is presently 10 pT s 1/2 , precluding potential applications in medical imaging, geoscience, and navigation. Here we show that high-permeability magnetic flux concentrators, which collect magnetic flux from a larger area and concentrate it into the diamond sensor, can be used to improve the sensitivity of diamond magnetometers. By inserting an NV-doped diamond membrane between two ferrite cones in a bowtie configuration, we realize a ∼250-fold increase of the magnetic field amplitude within the diamond. We demonstrate a sensitivity of ∼0.9 pT s 1/2 to magnetic fields in the frequency range between 10 and 1000 Hz. This is accomplished using a dual-resonance modulation technique to suppress the effect of thermal shifts of the NV spin levels. The magnetometer uses 200 mW of laser power and 20 mW of microwave power. This work introduces a new degree of freedom for the design of diamond sensors by using structured magnetic materials to manipulate magnetic fields.
Quantum sensors based on nitrogen-vacancy centers in diamond have emerged as a promising detection modality for nuclear magnetic resonance (NMR) spectroscopy owing to their micrometer-scale detection volume and noninductive-based detection. A remaining challenge is to realize sufficiently high spectral resolution and concentration sensitivity for multidimensional NMR analysis of picoliter sample volumes. Here, we address this challenge by spatially separating the polarization and detection phases of the experiment in a microfluidic platform. We realize a spectral resolution of 0.65 ± 0.05 Hz, an order-of-magnitude improvement over previous diamond NMR studies. We use the platform to perform two-dimensional correlation spectroscopy of liquid analytes within an effective ∼40-picoliter detection volume. The use of diamond quantum sensors as in-line microfluidic NMR detectors is a major step toward applications in mass-limited chemical analysis and single-cell biology.
Molecular-level insights into the entangled dynamics of high-molecular-weight chains, in particular of slower chain modes in regimes II−IV of the tube model, are still rare due to the lack of methods resolving the rather long associated time scales. On the theoretical side, new computer simulation methods are just reaching the relevant time scales in sufficiently large systems. Here, we confront results from a recent multiple-quantum proton NMR method with results from a novel lattice model. We address the concern that proton NMR, relying on the dipole−dipole couplings between nearby nuclei, is intrinsically sensitive not only to intrachain rotational motions which reflect the desired details of the tube model or possibly necessary modifications, but also to the translational diffusion of chains past each other via interchain dipole−dipole couplings. In order to critically assess the influence of the latter, we here present results of isotope-dilution experiments, in which the data reflect mainly tagged-chain dynamics. We find overall weak effects of interchain dipole−dipole couplings on the shape of the extracted orientation autocorrelation function and very good agreement of the experimental and the computer simulation data. We conclude that the NMR method as well as the novel lattice model faithfully reflects the universal features of entangled chain dynamics and in particular the deviations from simple tube-model predictions on a microscopic level.
Zeolite-catalyzed alkane C–H bond activation reactions carried out at room temperature, low pressure, and low reagent loadings demonstrate that water can act either to increase or to suppress the observed reaction rates. Isobutane-d10 undergoes hydrogen/deuterium exchange with the acidic zeolite HZSM-5 at subambient temperatures, as first reported by us (Truitt et al. J. Am. Chem. Soc. 2004, 126, 11144 and Truitt et al. J. Am. Chem. Soc. 2006, 128, 1847 ). New experiments demonstrate that the C–H bond activation chemistry is very sensitive to the presence of water. Isobutane reaction rate constants increase by an order of magnitude at water loadings in the range of ≤1 water molecule per catalyst active site relative to the dry catalyst. Conversely, water loadings greater than about 1–3 water molecules per active site retard isobutane reaction. In situ solid-state NMR data show that water molecules and isobutane molecules are simultaneously proximate to the catalyst active site. These results indicate that water can be an active participant in reactions involving hydrophobic molecules in solid acid catalysts, possibly via transition state stabilization, as long as the water concentration is essentially stoichiometric. Such conditions exist in well-known catalytic reactions, e.g., methanol-to-hydrocarbon chemistries, since stoichiometric water is a first-formed byproduct.
A comprehensive minimalistic model for spontaneous structural transition that is governed by distinct molecular interactions.
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