Application of nuclear magnetic resonance (NMR) spectroscopy to nanoscale samples has remained an elusive goal, achieved only with great experimental effort at subkelvin temperatures. We demonstrated ...detection of NMR signals from a (5-nanometer)(3) voxel of various fluid and solid organic samples under ambient conditions. We used an atomic-size magnetic field sensor, a single nitrogen-vacancy defect center, embedded ~7 nanometers under the surface of a bulk diamond to record NMR spectra of various samples placed on the diamond surface. Its detection volume consisted of only 10(4) nuclear spins with a net magnetization of only 10(2) statistically polarized spins.
The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, ...but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Further, slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the transfer protocol suggest slower molecular dynamics near the diamond surface compared to that in bulk. This observation is consistent with present models of the microscopic structure of a fluid and can be exploited to estimate the diffusion coefficient near a solid–liquid interface, of importance in colloid science.
Dynamic nuclear polarization (DNP) has enabled enormous gains in magnetic resonance signals and led to vastly accelerated NMR/MRI imaging and spectroscopy. Unlike conventional cw-techniques, DNP ...methods that exploit the full electron spectrum are appealing since they allow direct participation of all electrons in the hyperpolarization process. Such methods typically entail sweeps of microwave radiation over the broad electron linewidth to excite DNP but are often inefficient because the sweeps, constrained by adiabaticity requirements, are slow. In this paper, we develop a technique to overcome the DNP bottlenecks set by the slow sweeps, using a swept microwave frequency comb that increases the effective number of polarization transfer events while respecting adiabaticity constraints. This allows a multiplicative gain in DNP enhancement, scaling with the number of comb frequencies and limited only by the hyperfine-mediated electron linewidth. We demonstrate the technique for the optical hyperpolarization of 13C nuclei in powdered microdiamonds at low fields, increasing the DNP enhancement from 30 to 100 measured with respect to the thermal signal at 7T. For low concentrations of broad linewidth electron radicals e.g., TEMPO ((2,2,6,6-tetramethylpiperidin-1-yl)oxyl), these multiplicative gains could exceed an order of magnitude.
Diamond is a proven solid-state platform for spin-based quantum technology. The nitrogen-vacancy center in diamond has been used to realize small-scale quantum information processing and quantum ...sensing under ambient conditions. A major barrier in the development of large-scale quantum information processing in diamond is the connection of nitrogen-vacancy spin registers by a quantum bus at room temperature. Given that diamond is expected to be an ideal spin transport material, the coherent transport of spin directly between the spin registers offers a potential solution. Yet, there has been no demonstration of spin transport in diamond due to difficulties in achieving spin injection and detection via conventional methods. Here, we exploit detailed knowledge of the paramagnetic defects in diamond to identify novel mechanisms to photoionize, transport, and capture spin-polarized electrons in diamond at room temperature. Having identified these mechanisms, we explore how they may be combined to realize an on-chip spin quantum bus.
The origins of spin lifetimes in quantum systems is a matter of importance in several areas of quantum information. Spectrally mapping spin relaxation processes provides insight into their origin and ...motivates methods to mitigate them. In this paper, we map nuclear relaxation in a prototypical system of Formula: see text nuclei in diamond coupled to Nitrogen Vacancy (NV) centers over a wide field range (1 mT-7 T). Nuclear hyperpolarization through optically pumped NV electrons allows signal measurement savings exceeding million-fold over conventional methods. Through a systematic study with varying substitutional electron (P1 center) and Formula: see text concentrations, we identify the operational relaxation channels for the nuclei at different fields as well as the dominant role played by Formula: see text coupling to the interacting P1 electronic spin bath. These results motivate quantum control techniques for dissipation engineering to boost spin lifetimes in diamond, with applications including engineered quantum memories and hyperpolarized Formula: see text imaging.
We demonstrate a protocol using individual nitrogen-vacancy centres in diamond to observe the time evolution of proton spins from organic molecules located a few nanometres from the diamond surface. ...The protocol records temporal correlations among the interacting protons, and thus is sensitive to the local dynamics via its impact on the nuclear spin relaxation and interaction with the nitrogen vacancy. We gather information on the nanoscale rotational and translational diffusion dynamics by analysing the time dependence of the nuclear magnetic resonance signal. Applying this technique to liquid and solid samples, we find evidence that liquid samples form a semi-solid layer of 1.5-nm thickness on the surface of diamond, where translational diffusion is suppressed while rotational diffusion remains present. Extensions of the present technique could be exploited to highlight the chemical composition of molecules tethered to the diamond surface or to investigate thermally or chemically activated dynamical processes such as molecular folding.
This work analyzes the direct effect of soil management practices on soil microbial communities, which may affect soil productivity and sustainability. The experimental design consisted of two ...tillage treatments: reduced tillage (RT) and zero tillage (ZT), and three crop rotation treatments: continuous soybean (SS), corn–soybean (CS), and soybean–corn (SC). Soil samples were taken at soybean planting and harvest. The following quantifications were performed: soil microbial populations by soil dilution plate technique on selective and semi-selective culture media; microbial respiration and microbial biomass by chloroform fumigation-extraction; microbial activity by fluorescein diacetate hydrolysis; and fatty acid methyl ester (FAME) profiles. Soil chemical parameters were also quantified. Soil organic matter content was significantly lower in RT and SS sequence crops, whereas soil pH and total N were significantly higher in CS and SC sequence crops.
Trichoderma and
Gliocladium populations were lower under RTSS and ZTSS treatments. Except in a few cases, soil microbial respiration, biomass and activity were higher under zero tillage than under reduced tillage, both at planting and harvest sampling times. Multivariate analyses of FAMEs clearly separated both RT and ZT management practices at each sampling time; however, separation of sequence crops was less evident. In our experiments ZT treatment had highest proportion of 10Me 16:0, an actinomycetes biomarker, and 16:1ω9 and 18:1ω7, two fatty acids associated with organic matter content and substrate availability. In contrast, RT treatment had highest content of branched biomarkers (i15:0 and i16:0) and of cy19:0, fatty acids associated with cell stasis and/or stress. As cultural practices can influence soil microbial populations, it is important to analyze the effect that they produce on biological parameters, with the aim of conserving soil richness over time. Thus, in a soybean-based cropping system, appropriate crop management is necessary for a sustainable productivity without reducing soil quality.
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•Exposition of the DNP mechanism for 13C nuclei in optically pumped diamond with a focus on multi-nuclear Landau–Zener crossings•Features of the DNP mechanism in orientation ...independence.•New “Hole burning” DNP protocol for high resolution DNP-ESR spectroscopy.
The emergence of a new class of optically polarizable electronic spins in diamond, nitrogen vacancy (NV) defect centers, has opened interesting new avenues for dynamic nuclear polarization. Here we review methods for the room-temperature hyperpolarization of lattice 13C nuclei using optically pumped NV centers, focusing particular attention to a polarization transfer via rotating-frame level anti-crossings. We describe special features of this optical dynamic nuclear polarization (DNP) mechanism at low-field, in particular, its deployability to randomly oriented diamond nanoparticles. In addition, we detail methods for indirectly obtaining high-resolution NV ESR spectra via hyperpolarization readout. These mechanistic features provide perspectives for interesting new applications exploiting the optically generated 13C hyperpolarization.
The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, ...however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV‒, on the other hand, yields only fractional recombination into SiV2‒, a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.
Silicon vacancy (SiV) centers in diamond are candidates for quantum networks but exhibit charge instability under illumination. This work uses variable‐wavelength infra‐red excitation to characterize charge transfer from SiV0 to SiV− and from SiV− to SiV2−. These processes occur via different mechanisms, namely, single‐photon recombination and electron tunnelling from a nitrogen donor, findings supported by density functional theory modeling.
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