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Results for “nuclear spin resonance”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Vanadium spin qubits as telecom quantum emitters in silicon carbide

Solid-state quantum emitters with spin registers are promising platforms for quantum communication, yet few emit in the narrow telecom band necessary for low-loss fiber networks. Here, we create and isolate near-surface single vanadium dopants in silicon carbide (SiC) with stable and narrow emission in the O band, with brightness allowing cavity-free detection in a wafer-scale material. In vanadium ensembles, we characterize the complex d 1 orbital physics in all five available sites in 4H-SiC and 6H-SiC. The optical transitions are sensitive to mass shifts from local silicon and carbon isotopes, enabling optically resolved nuclear spin registers. Optically detected magnetic resonance in the ground and excited orbital states reveals a variety of hyperfine interactions with the vanadium nuclear spin and clock transitions for quantum memories. Last, we demonstrate coherent quantum control of the spin state. These results provide a path for telecom emitters in the solid state for quantum applications.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Toward Ultra‐High‐Quality‐Factor Wireless Masing Magnetic Resonance Sensing

It has recently been shown that a bolus of hyperpolarized nuclear spins can yield stimulated emission signals similar in nature to maser signals, potentially enabling new ways of sensing hyperpolarized contrast media, including most notably [1- 13 C]pyruvate that is under evaluation in over 50 clinical trials for metabolic imaging of cancer. The stimulated NMR signal emissions lasting for minutes do not require radio-frequency excitation, offering unprecedented advantages compared to conventional MR sensing. However, creating nuclear spin maser emission is challenging in practice due to stringent fundamental requirements, making practical in vivo applications hardly possible using conventional passive MR detectors. Here, in this study, we demonstrate the utility of a wireless NMR maser detector, the quality factor of which was enhanced 22-fold (to 1,670) via parametric pumping. This active-feedback technique breaks the intrinsic fundamental limit of NMR detector circuit quality factor. We show the use of parametric pumping to reduce the threshold requirement for inducing nuclear spin masing at 300 MHz resonance frequency in a preclinical MRI scanner. Indeed, stimulated emission from hyperpolarized protons was obtained under highly unfavorable conditions of low magnetic field homogeneity (T 2 * of 3 ms). Greater gains of the quality factor of the MR detector (up to 1 million) were also demonstrated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Protecting air/moisture-sensitive samples using perdeuterated paraffin wax for solid-state NMR experiments under magic-angle spinning

Solid-state nuclear magnetic resonance (SSNMR) spectroscopy is a powerful technique for materials characterization, yet its application to air- and moisture-sensitive materials is often hindered by the difficulty in maintaining an inert environment during magic-angle spinning (MAS). This is particularly true for fast-MAS rotors that do not generally provide tight seals. Herein, we present a generalizable approach employing perdeuterated paraffin waxes—n-icosane-d42 and c-dodecane-d24—as protective embedding media to analyze sensitive organometallic catalysts using SSNMR. We demonstrate that these waxes significantly slow oxidative degradation under MAS conditions. Weak background 1 H and 13 C NMR signals from the waxes are effectively suppressed using double-quantum filtration and cross-polarization techniques. In conclusion, these findings offer a robust method for expanding the scope of SSNMR to air-sensitive systems, with implications for the structural study of reactive materials and catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Automating neutron resonances classification with Machine Learning [Slides]

Team reported the following accomplishments: the development of a Machine-Learning method to properly assign spins to neutron resonances (automated, general, reproducible); full integration with evaluated resonances in the Atlas (automation of new editions); training and optimization in synthetic data; validation and deployment to real experimental resonances. Future perspectives include exploration of other classifiers and hyper-parameter combinations, further validation with well-known nucleus (e.g. 235 U), and publication pipeline.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Microsized Pore Structure Determination in EPDM Rubbers Using High-Pressure 129 Xe NMR Techniques

Microsized pore parameters, such as pore size and distance between pores in a series of model EPDM rubbers, were determined in situ under the pressure of 500 psi using 129 Xe nuclear magnetic resonance (NMR) techniques: spin–lattice (T 1 ) and spin–spin (T 2 ) relaxation measurements, pulsed-field gradient (PFG) NMR, and two-dimensional exchange spectroscopy (2D EXSY). The T 1 /T 2 (>>1) ratio for the xenon confined in the pores is larger than that for nonconfined free xenon. This suggests that almost the entire pore surface interacts with xenon atoms like a closed pore. While these pores still connect each other through very narrow diffusion/exchange channels, it is possible to observe the echo decay in PFG-NMR and cross-peaks in 2D EXSY. The results show that both diffusion (D pore ≈ 2.1 × 10 –10 m 2 /s) and exchange (exchange rate, τ exch = a few tens of milliseconds) of xenon between a pore within the material and outer surface are prolonged. The exchange distances (l), which correspond to the xenon gas penetration depth, were estimated to be 70–100 μm based on the measured diffusion coefficients and exchange rate (1/τ exch ). NMR diffraction analysis reveals that pore size (a) and pore distance (b) are on the order of magnitude of micrometers and tens of micrometers, while the diffusion coefficients of xenon gas in the diffusion channels (D eff ) are about 10 –8 m 2 /s. Overall, this study suggests that the pores with a few micrometers connected through very narrow flowing channels with the length of several tens of micrometers are developed 70 to 100 μm below the rubber surface. Furthermore, the overall steady-state diffusion of xenon is slower, approximately 2 orders of magnitudes, than the diffusion in the channel between the pores. Finally, the pore and exchange distances correlated with the composition of rubbers showed that the properties of EPDM rubber as a high-pressure gas barrier could be improved by reducing the size of cracks and the depth of gas penetration by the addition of both carbon black and silica fillers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Carbon-13 Radiofrequency Amplification by Stimulated Emission of Radiation of the Hyperpolarized Ketone and Hemiketal Forms of Allyl [1- 13 C]Pyruvate

13 C hyperpolarized pyruvate is an emerging MRI contrast agent for sensing molecular events in cancer and other diseases with aberrant metabolic pathways. This metabolic contrast agent can be produced via several hyperpolarization techniques. Despite remarkable success in research settings, widespread clinical adoption faces substantial roadblocks because the current sensing technology utilized to sense this contrast agent requires the excitation of 13 C nuclear spins that also need to be synchronized with MRI field gradient pulses. Here, we demonstrate sensing of hyperpolarized allyl [1- 13 C]pyruvate via the stimulated emission of radiation that mitigates the requirements currently blocking broader adoption. Specifically, 13 C Radiofrequency Amplification by Stimulated Emission of Radiation ( 13 C RASER) was obtained after pairwise addition of parahydrogen to a pyruvate precursor, detected in a commercial inductive detector with a quality factor (Q) of 32 for sample concentrations as low as 0.125 M with 13 C polarization of 4%. Moreover, parahydrogen-induced polarization allowed for the preparation of a mixture of ketone and hemiketal forms of hyperpolarized allyl [1- 13 C]pyruvate, which are separated by 10 ppm in 13 C NMR spectra. This is a good model system to study the simultaneous 13 C RASER signals of multiple 13 C species. This system models the metabolic production of hyperpolarized [1- 13 C]lactate from hyperpolarized [1- 13 C]pyruvate, which has a similar chemical shift difference. Our results show that 13 C RASER signals can be obtained from both species simultaneously when the emission threshold is exceeded for both species. On the other hand, when the emission threshold is exceeded only for one of the hyperpolarized species, 13 C stimulated emission is confined to this species only, therefore enabling the background-free detection of individual hyperpolarized 13 C signals. Furthermore, the reported results pave the way to novel sensing approaches of 13 C hyperpolarized pyruvate, potentially unlocking hyperpolarized 13 C MRI on virtually any MRI system–an attractive vision for the future molecular imaging and diagnostics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Novel machine-learning method for spin classification of neutron resonances

The performance of nuclear reactors and other nuclear systems depends on a precise understanding of the neutron interaction cross sections for materials used in these systems. These cross sections exhibit resonant structure whose shape is determined in part by the angular-momentum quantum numbers of the resonances. The correct assignment of the quantum numbers of neutron resonances is, therefore, paramount. In this project, we apply machine learning to automate the quantum number assignments using only the resonances' energies and widths and not relying on detailed transmission or capture measurements. The classifier used for quantum number assignment is trained using stochastically generated resonance sequences whose distributions mimic those of real data. Here we explore the use of several physics-motivated features for training our classifier. These features amount to out-of-distribution tests of a given resonance's widths and resonance-pair spacings. We pay special attention to situations where either capture widths cannot be trusted for classification purposes or where there is insufficient information to classify resonances by the total spin J. We demonstrate the efficacy of our classification approach using simulated and actual 52 Cr resonance data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Magnetic properties of a spin-orbit entangled $J_{eff}$ = $\frac{1}{2}$ honeycomb lattice

The interplay between spin-orbit coupling, anisotropic magnetic interaction, frustration-induced quantum fluctuations, and spin correlations can lead to novel quantum states with exotic excitations in rare-earth-based quantum magnets. Herein, we present the crystal structure, magnetization, electron spin resonance (ESR), specific heat, and nuclear magnetic resonance (NMR) experiments on the polycrystalline samples of $\mathrm{Ba_9}$$\mathrm{Yb_2}$$\mathrm{Si_6}$$\mathrm{O_{24}}$, in which $\mathrm{Yb^{3+}}$ ions form a perfect honeycomb lattice without detectable antisite disorder. The magnetization data reveal antiferromagnetically coupled spin-orbit entangled $J_{eff}$ = $\frac{1}{2}$ degrees of freedom of $\mathrm{Yb^{3+}}$ ions in the Kramers doublet state. The ESR measurements reveal that the first excited Kramers doublet is 32.3(7) meV above the ground state. The specific heat results suggest the absence of any long-range magnetic order in the measured temperature range. Furthermore, the $\mathrm{^{29}Si}$ NMR results do not indicate any signature of magnetic ordering down to 1.6 K, and the spin-lattice relaxation rate reveals the presence of a field-induced gap that is attributed to the Zeeman splitting of the Kramers doublet state in this quantum material. Here, our experiments detect neither spin freezing nor long-range magnetic ordering down to 1.6 K. The current results suggest the presence of short-range spin correlations in this spin-orbit entangled $J_{eff}$ = $\frac{1}{2}$ rare-earth magnet on a honeycomb lattice.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Role of Nematic Fluctuations on Superconductivity in FeSe 0.47 ⁢Te 0.53 Revealed by Nuclear Magnetic Resonance under Pressure

The relationship between antiferromagnetic (AFM) spin fluctuations (SF), nematic fluctuations, and superconductivity (SC) has been central to understanding the pairing mechanism in iron-based superconductors (IBSCs). Iron chalcogenides, which hold the simplest crystal structure in IBSCs, provide a good platform to investigate the relationship. Here, we report 77 Se and 125 Te nuclear magnetic resonance studies of FeSe 0.47⁢ Te 0.53 , which is located close to a nematic quantum critical point (QCP), under pressures up to 1.35 GPa. Further, both the superconducting critical temperature and AFMSF were found to be enhanced under pressure, which suggests a correlation between SC and AFMSF in FeSe 0.47 ⁢Te 0.53 . However, the contribution of AFMSF to SC in FeSe 0.47 ⁢Te 0.53 was found to be much less compared to that in FeSe 1−𝑥 ⁢S 𝑥 , suggesting that nematic fluctuations play a dominant role in the SC in FeSe 1−𝑥⁢ Te 𝑥 around the nematic QCP.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via 161 Dy Nuclear Resonance Vibrational Spectroscopy

Synchrotron-based nuclear resonance vibrational spectroscopy (NRVS) using the Mossbauer isotope 161 Dy has been employed for the first time to study the vibrational properties of a single-molecule magnet (SMM) incorporating Dy III , namely [Dy(Cy3PO)(2)(H2O)(5)]Br-3•2 (Cy3PO)•2 H2O•2 EtOH. The experimental partial phonon density of states (pDOS), which includes all vibrational modes involving a displacement of the Dy III ion, was reproduced by means of simulations using density functional theory (DFT), enabling the assignment of all intramolecular vibrational modes. This study proves that 161 Dy NRVS is a powerful experimental tool with significant potential to help to clarify the role of phonons in SMMs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Nuclear spin conservation enables state-to-state control of ultracold molecular reactions

Quantum-state control of reactive systems has enabled microscopic probes of underlying interaction potentials and the alteration of reaction rates using quantum statistics. However, extending such control to the quantum states of reaction outcomes remains challenging. Here in this work, we realize this goal by utilizing the conservation of nuclear spins throughout the reaction. Using resonance-enhanced multiphoton ionization spectroscopy to investigate the products formed in bimolecular reactions between ultracold KRb molecules we find that the system retains a near-perfect memory of the reactants’ nuclear spins, manifested as a strong parity preference for the rotational states of the products. We leverage this effect to alter the occupation of these product states by changing the coherent superposition of initial nuclear spin states with an external magnetic field. In this way, we are able to control both the inputs and outputs of a reaction with quantum-state resolution. The techniques demonstrated here open up the possibilities to study quantum entanglement between reaction products, and ultracold reaction dynamics at the state-to-state level.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Frequency‐Scanning Considerations in Axionlike Dark Matter Spin‐Precession Experiments

Abstract Galactic dark matter may consist of axionlike particles (ALPs) that can be described as an “ultralight bosonic field” oscillating at the ALP Compton frequency. The ALP field can be searched for using nuclear magnetic resonance (NMR), where resonant precession of spins of a polarized sample can be sensitively detected. The ALP mass to which the experiment is sensitive is scanned by sweeping the bias magnetic field. The scanning either results in detection of ALP dark matter or rules out ALP dark matter with sufficiently strong couplings to nuclear spins over the range of ALP masses corresponding to the covered span of Larmor frequencies. In this work, scanning strategies are analyzed with the goal of optimizing the parameter‐space coverage via a proper choice of experimental parameters (e.g., the effective transverse relaxation time).

Zhang, Yuzhe (ORCID:0009000660829066)↗
DOE OSTI2021

One-directional polarization transport in electron/nuclear spin chains with loss and gain

Understanding the joint dynamics of electron and nuclear spins is central to core concepts in solid-state magnetic resonance such as spin-lattice relaxation and dynamic nuclear polarization, but a generalization that capitalizes on competing polarization loss and gain channels is still lacking. Here, we study theoretically the non-Hermitian dynamics of hybrid electron/nuclear spin systems in the simultaneous presence of electron spin pumping and spin-lattice relaxation. Focusing on periodic, one-dimensional chains, we find that, by adjusting the electron spin pumping to a critical level, it is possible to steer the flow of nuclear polarization to create site-dependent distributions where either end of the array polarizes in opposite ways, irrespective of the initial state. By contrast, we show that ring-like patterns—where the limit nuclear polarization is uniform—exhibit a non-decaying, externally driven nuclear spin current. Interestingly, cyclic magnetic field modulation can render these processes largely robust to defects in the chain, a response featuring some interesting similarities—and differences—with recent findings in other non-Hermitian physical platforms.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Enhanced Softwood Cellulose Accessibility by H 3 PO 4 Pretreatment: High Sugar Yield without Compromising Lignin Integrity

Softwood lignocellulose is a potential feedstock for the production of biofuels and bioproducts. However, the highly cross-linked nature of softwood lignocellulose restricts enzyme access to its sugars. Thus, harsh pretreatment conditions (180–280 °C) and/or high enzyme loading are required to unlock sugars. These requirements negatively affect the economic viability of softwoods in biorefineries. Here we show that H 3 PO 4 pretreatment of pine and Douglas fir under a mild reaction temperature (50 °C) and atmospheric pressure enabled a high (~80%) glucan digestibility with low enzyme loading (5 filter paper units (FPU)/g glucan). The dissolution and regeneration of softwoods disrupted the hydrogen bonding between cellulose chains, thereby increasing the cellulose accessibility to cellulase (CAC) values by ~38-fold (from ~0.4 to 15 m 2 /g biomass). Examination of H 3 PO 4 -pretreated softwoods by cross-polarization/magic angle spin (CP/MAS), 13 C- nuclear magnetic resonance (NMR), and Fourier-transform infrared spectroscopy (FTIR) revealed that breaking of the orderly hydrogen bonding of crystalline cellulose caused the increase in CAC (higher than 11 m 2 /g biomass), which, in turn, was responsible for the high glucan digestibility of pretreated softwoods. The H 3 PO 4 pretreatment process was feedstock independent. Finally, 2D 13 C– 1 H heteronuclear single quantum coherence (HSQC) NMR showed that the lignin was depolymerized but not condensed; thus, the lignin can be available for producing high-value products.

09 BIOMASS FUELS↗
DOE OSTI2022

Enhanced Catalytic Performance of a Ce/V Oxo Cluster through Confinement in Mesoporous SBA-15

To increase catalytic efficiency, mesoporous supports have been widely applied to immobilize well-defined metal oxide clusters due to their ability to stabilize highly dispersed clusters. Here, for this study, a redox-active heterometallic Ce 12 V 6 -oxo cluster (CeV) was first presynthesized and then incorporated into mesoporous silica, SBA-15, via a straightforward impregnation method. Scanning transmission electron microscopy (STEM) and Fourier transform infrared spectroscopy (FTIR), in concert with scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM-EDS), verified the successful introduction of the CeV cluster inside the pore of SBA-15. The 51 V magic angle spinning solid-state nuclear magnetic resonance ( 51 V MAS NMR) spectroscopy and differential pair distribution function (dPDF) analysis confirmed the structural integrity of the CeV cluster inside the SBA-15. The composite was then benchmarked for liquid-phase oxidation of 2-chloroethyl ethyl sulfide (CEES) under mild conditions and gas-phase oxidative dehydrogenation (ODH) of propane under high temperatures (up to 550 °C). The catalytic reactivity results demonstrated 8- and 14-fold increase in turnover frequency (TOF) values of the composite (CeV@10SBA-2) than the bulk CeV cluster under the same conditions for CEES oxidation and ODH, respectively. These results highlight the improved reactivity of the catalytically active CeV cluster as attributed to the higher dispersion of the discrete cluster upon immobilization within the SBA-15 support.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Universal fluctuating regime in triangular chromate antiferromagnets

In this work, we report x-ray diffraction, magnetic susceptibility, heat capacity, 1 H nuclear magnetic resonance (NMR), and muon spin relaxation (μSR) measurements, as well as density-functional band-structure calculations for the frustrated S=3/2 triangular lattice Heisenberg antiferromagnet (TLHAF) α-HCrO 2 (trigonal, space group: $R\bar{3}m$). This compound undergoes a clear magnetic transition at T N ≃22.5 K, as seen from the drop in the muon paramagnetic fraction and concurrent anomalies in the magnetic susceptibility and specific heat capacity. Local probes (NMR and μSR) reveal a broad regime with slow fluctuations down to 0.7T N , this temperature corresponding to the maximum in the μSR relaxation rate and in the NMR wipe-out. From the comparison with NaCrO 2 and α-KCrO 2 , the fluctuating regime and slow dynamics below T N appear to be hallmarks of the TLHAF with ABC stacking. We discuss the role of interlayer frustration, which may have impacted recent spin-liquid candidates with triangular geometry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗