47 research outputs found
Enhanced dynamic nuclear polarization via swept microwave frequency combs
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, employing 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, these multiplicative gains could exceed an order of
magnitude.Comment: Contains supplementary inf
Room temperature "optical nanodiamond hyperpolarizer": Physics, design, and operation.
Dynamic Nuclear Polarization (DNP) is a powerful suite of techniques that deliver multifold signal enhancements in nuclear magnetic resonance (NMR) and MRI. The generated athermal spin states can also be exploited for quantum sensing and as probes for many-body physics. Typical DNP methods require the use of cryogens, large magnetic fields, and high power microwave excitation, which are expensive and unwieldy. Nanodiamond particles, rich in Nitrogen-Vacancy (NV) centers, have attracted attention as alternative DNP agents because they can potentially be optically hyperpolarized at room temperature. Here, unraveling new physics underlying an optical DNP mechanism first introduced by Ajoy et al. [Sci. Adv. 4, eaar5492 (2018)], we report the realization of a miniature "optical nanodiamond hyperpolarizer," where 13C nuclei within the diamond particles are hyperpolarized via the NV centers. The device occupies a compact footprint and operates at room temperature. Instrumental requirements are very modest: low polarizing fields, low optical and microwave irradiation powers, and convenient frequency ranges that enable miniaturization. We obtain the best reported optical 13C hyperpolarization in diamond particles exceeding 720 times of the thermal 7 T value (0.86% bulk polarization), corresponding to a ten-million-fold gain in averaging time to detect them by NMR. In addition, the hyperpolarization signal can be background-suppressed by over two-orders of magnitude, retained for multiple-minute long periods at low fields, and deployed efficiently even to 13C enriched particles. Besides applications in quantum sensing and bright-contrast MRI imaging, this work opens possibilities for low-cost room-temperature DNP platforms that relay the 13C polarization to liquids in contact with the high surface-area particles
Enhanced Optical 13C Hyperpolarization in Diamond Treated by High-Temperature Rapid Thermal Annealing
Methods of optical dynamic nuclear polarization open the door to the replenishable hyperpolarization of nuclear spins, boosting their nuclear magnetic resonance/imaging signatures by orders of magnitude. Nanodiamond powder rich in negatively charged nitrogen vacancy defect centers has recently emerged as one such promising platform, wherein 13C nuclei can be hyperpolarized through the optically pumped defects completely at room temperature. Given the compelling possibility of relaying this 13C polarization to nuclei in external liquids, there is an urgent need for the engineered production of highly “hyperpolarizable” diamond particles. Here, a systematic study of various material dimensions affecting optical 13C hyperpolarization in diamond particles is reported on. It is discovered surprisingly that diamond annealing at elevated temperatures ∼1720 °C has remarkable effects on the hyperpolarization levels enhancing them by above an order of magnitude over materials annealed through conventional means. It is demonstrated these gains arise from a simultaneous improvement in NV− electron relaxation/coherence times, as well as the reduction of paramagnetic content, and an increase in 13C relaxation lifetimes. This work suggests methods for the guided materials production of fluorescent, 13C hyperpolarized, nanodiamonds and pathways for their use as multimodal (optical and magnetic resonance) imaging and hyperpolarization agents
Wide dynamic range magnetic field cycler: Harnessing quantum control at low and high fields
We describe the construction of a fast field cycling device capable of
sweeping a 4-order-of-magnitude range of magnetic fields, from ~1mT to 7T, in
under 700ms. Central to this system is a high-speed sample shuttling mechanism
between a superconducting magnet and a magnetic shield, with the capability to
access arbitrary fields in between with high resolution. Our instrument serves
as a versatile platform to harness the inherent dichotomy of spin dynamics on
offer at low and high fields - in particular, the low anisotropy, fast spin
manipulation, and rapid entanglement growth at low field as well as the long
spin lifetimes, spin specific control, and efficient inductive measurement
possible at high fields. Exploiting these complementary capabilities in a
single device open up applications in a host of problems in quantum control,
sensing, and information storage, besides in nuclear hypepolarization,
relaxometry and imaging. In particular, in this paper, we focus on the ability
of the device to enable low-field hyperpolarization of 13C nuclei in diamond
via optically pumped electronic spins associated with Nitrogen Vacancy (NV)
defect centers
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High contrast dual-mode optical and 13C magnetic resonance imaging in diamond particles
Multichannel imaging -- the ability to acquire images of an object through
more than one imaging mode simultaneously -- has opened interesting new
perspectives in areas ranging from astronomy to medicine. Visible optics and
magnetic resonance imaging (MRI) offer complementary advantages of resolution,
speed and depth of penetration, and as such would be attractive in combination.
In this paper, we take first steps towards marrying together optical and MR
imaging in a class of biocompatible particulate materials constructed out of
diamond. The particles are endowed with a high density of quantum defects
(Nitrogen Vacancy centers) that under optical excitation fluoresce brightly in
the visible, but also concurrently electron spin polarize. This allows the
hyperpolarization of lattice 13C nuclei to make the particles over three-orders
of magnitude brighter than in conventional MRI. Dual-mode optical and MR
imaging permits immediate access to improvements in resolution and
signal-to-noise especially in scattering environments. We highlight additional
benefits in background-free imaging, demonstrating lock-in suppression by
factors of 2 and 5 in optical and MR domains respectively. Ultimate limits
could approach as much as two orders of magnitude in each domain. Finally,
leveraging the ability of optical and MR imaging to simultaneously probe
Fourier-reciprocal domains (real and k-space), we elucidate the ability to
employ hybrid sub-sampling in both conjugate spaces to vastly accelerate
dual-image acquisition, by as much as two orders of magnitude in practically
relevant sparse-imaging scenarios. This is accompanied by a reduction in
optical power by the same factor. Our work suggests interesting possibilities
for the simultaneous optical and low-field MR imaging of targeted diamond
nanoparticles
Evidence of Key Tinnitus-Related Brain Regions Documented by a Unique Combination of Manganese-Enhanced MRI and Acoustic Startle Reflex Testing
Animal models continue to improve our understanding of tinnitus pathogenesis and aid in development of new treatments. However, there are no diagnostic biomarkers for tinnitus-related pathophysiology for use in awake, freely moving animals. To address this disparity, two complementary methods were combined to examine reliable tinnitus models (rats repeatedly administered salicylate or exposed to a single noise event): inhibition of acoustic startle and manganese-enhanced MRI. Salicylate-induced tinnitus resulted in wide spread supernormal manganese uptake compared to noise-induced tinnitus. Neither model demonstrated significant differences in the auditory cortex. Only in the dorsal cortex of the inferior colliculus (DCIC) did both models exhibit supernormal uptake. Therefore, abnormal membrane depolarization in the DCIC appears to be important in tinnitus-mediated activity. Our results provide the foundation for future studies correlating the severity and longevity of tinnitus with hearing loss and neuronal activity in specific brain regions and tools for evaluating treatment efficacy across paradigms
Orientation-independent room temperature optical C-13 hyperpolarization in powdered diamond
Dynamic nuclear polarization via contact with electronic spins has emerged as an attractive route to enhance the sensitivity of nuclear magnetic resonance beyond the traditional limits imposed by magnetic field strength and temperature. Among the various alternative implementations, the use of nitrogen vacancy (NV) centers in diamond—a paramagnetic point defect whose spin can be optically polarized at room temperature—has attracted widespread attention, but applications have been hampered by the need to align the NV axis with the external magnetic field. We overcome this hurdle through the combined use of continuous optical illumination and a microwave sweep over a broad frequency range. As a proof of principle, we demonstrate our approach using powdered diamond with which we attain bulk 13C spin polarization in excess of 0.25% under ambient conditions. Remarkably, our technique acts efficiently on diamond crystals of all orientations and polarizes nuclear spins with a sign that depends exclusively on the direction of the microwave sweep. Our work paves the way toward the use of hyperpolarized diamond particles as imaging contrast agents for biosensing and, ultimately, for the hyperpolarization of nuclear spins in arbitrary liquids brought in contact with their surface
Post hoc immunostaining of GABAergic neuronal subtypes following in vivo two-photon calcium imaging in mouse neocortex
GABAergic neurons in the neocortex are diverse with regard to morphology, physiology, and axonal targeting pattern, indicating functional specializations within the cortical microcircuitry. Little information is available, however, about functional properties of distinct subtypes of GABAergic neurons in the intact brain. Here, we combined in vivo two-photon calcium imaging in supragranular layers of the mouse neocortex with post hoc immunohistochemistry against the three calcium-binding proteins parvalbumin, calretinin, and calbindin in order to assign subtype marker profiles to neuronal activity. Following coronal sectioning of fixed brains, we matched cells in corresponding volumes of image stacks acquired in vivo and in fixed brain slices. In GAD67-GFP mice, more than 95% of the GABAergic cells could be unambiguously matched, even in large volumes comprising more than a thousand interneurons. Triple immunostaining revealed a depth-dependent distribution of interneuron subtypes with increasing abundance of PV-positive neurons with depth. Most importantly, the triple-labeling approach was compatible with previous in vivo calcium imaging following bulk loading of Oregon Green 488 BAPTA-1, which allowed us to classify spontaneous calcium transients recorded in vivo according to the neurochemically defined GABAergic subtypes. Moreover, we demonstrate that post hoc immunostaining can also be applied to wild-type mice expressing the genetically encoded calcium indicator Yellow Cameleon 3.60 in cortical neurons. Our approach is a general and flexible method to distinguish GABAergic subtypes in cell populations previously imaged in the living animal. It should thus facilitate dissecting the functional roles of these subtypes in neural circuitry