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At least 19 records

Spin squeezing of macroscopic nuclear spin ensembles

Spin squeezing has been explored in atomic systems as a tool for quantum sensing, improving experimental sensitivity beyond the spin standard quantum limit for certain measurements. To optimize absolute metrological sensitivity, it is beneficial to consider macroscopic spin ensembles, such as nuclear spins in solids and liquids. Coupling a macroscopic spin ensemble to a parametrically-modulated resonant circuit can create collective spin squeezing by generating spin correlations mediated by the circuit. We analyze the squeezing dynamics in the presence of decoherence and finite spin polarization, showing that achieving 7 dB spin squeezing is feasible in several nuclear spin systems. The metrological benefit of squeezing a macroscopic spin ensemble lies in the suppression of technical noise sources in the spin detection system relative to the spin projection noise. This expands the experimental sensitivity bandwidth when searching for signals of unknown frequency and can improve the resonant signal-to-noise ratio. Squeezing macroscopic spin ensembles may prove to be a useful technique for fundamental physics experiments aimed at detecting spin interactions with oscillating background fields, such as ultralight dark matter. Published by the American Physical Society 2025

Boyers, Eric↗

High-Field One-Dimensional and Two-Dimensional 27Al Magic-Angle Spinning Nuclear Magnetic Resonance Study of ?-, d-, and ?-Al2O3 Dominated Aluminum Oxides: Toward Understanding the Al Sites in ?-Al2O3

Herein, a detailed analysis was carried out using high-field (19.9 T) 27Al magic-angle spinning (MAS) nuclear magnetic resonance (NMR) on three specially prepared aluminum oxide samples where the ?-, d-, and ?-Al2O3 phases are dominantly expressed through careful control of the synthesis conditions. Specifically, two-dimensional (2D) multiquantum (MQ) MAS 27Al was used to obtain high spectral resolution, which provided a guide for analyzing quantitative 1D 27Al NMR spectra. Six aluminum sites were resolved in the 2D MQ MAS NMR spectra, and seven aluminum sites were required to fit the 1D spectra. A set of octahedral and tetrahedral peaks with well-defined quadrupolar line shapes was observed in the ?-phase dominant sample and was unambiguously assigned to the ?-Al2O3 phase. The distinct line shapes related to the ?-Al2O3 phase provided an opportunity for effectively deconvoluting the more complex spectrum obtained from the d-Al2O3 dominant sample, allowing the peaks/quadrupolar parameters related to the d-Al2O3 phase to be extracted. The results show that the d-Al2O3 phase contains three distinct AlO sites and three distinct AlT sites. This detailed Al site structural information offers a powerful way of analyzing the most complex ?-Al2O3 spectrum. It is found that the ?-Al2O3 phase consists of Al sites with local structures similar to those found in the d-Al2O3 and ?-Al2O3 phases albeit with less ordering. Spin–lattice relaxation time measurement further confirms the disordering of the lattice. Collectively, this study uniquely assigns 27Al features in transition aluminas, offering a simplified method to quantify complex mixtures of aluminum sites in transition alumina samples.

Xu, Suochang↗

Dynamic Nuclear Polarization Enhanced Nuclear Spin Optical Rotation

Here, nuclear spin optical rotation (NSOR) has been investigated as a magneto-optical effect, which holds the potential for applications, including hybrid optical-nuclear magnetic resonance (NMR) spectroscopy and gradientless imaging. The intrinsic nature of NSOR renders its detection relatively insensitive, which has prevented it moving from a proof of concept to a method supporting chemical characterizations. In this work, the dissolution dynamic nuclear polarization technique is introduced to provide nuclear spin polarization, increasing the signal-to-noise ratio by several thousand times. NSOR signals of 1 H and 19 F nuclei are observed in a single scan for diluted compounds, which has made this effect suitable for the determination of electronic transitions from a specific nucleus in a large molecule.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Nuclear spin engineering for quantum information science

Semiconductors are the backbone of modern technology, garnering decades of investment in high-quality materials and devices. Electron spin systems in semiconductors, including atomic defects and quantum dots, have been demonstrated in the last two decades to host quantum coherent spin qubits, often with coherent spin–photon interfaces and proximal nuclear spins. These systems are at the center of developing quantum technology. However, new material challenges arise when considering the isotopic composition of host and qubit systems. The isotopic composition governs the nature and concentration of nuclear spins, which naturally occur in leading host materials. These spins generate magnetic noise—detrimental to qubit coherence—but also show promise as local quantum memories and processors, necessitating careful engineering dependent on the targeted application. Reviewing recent experimental and theoretical progress toward understanding local nuclear spin environments in semiconductors, we show this aspect of material engineering as critical to quantum information technology.

Defects↗

Entanglement of a nuclear spin qubit register in silicon photonics

Colour centres provide an optical interface to quantum registers based on electron and nuclear spin qubits in solids. The T centre in silicon is an emerging spin–photon interface that combines telecom O-band optical transitions and an electron spin in a scalable photonics platform. Here, in this study, we integrate T centres into single-mode photonic waveguides in a silicon-on-insulator platform. We demonstrate the initialization, coherent control and state read-out of a three-qubit register based on the electron spin of a T centre coupled to a hydrogen and a silicon nuclear spin. The spin register exhibits spin echo coherence times of 0.41(2) ms for the electron spin, 112(12) ms for the hydrogen nuclear spin and 67(7) ms for the silicon nuclear spin. We use nuclear–nuclear two-qubit gates to generate entanglement between the two nuclear spins with a fidelity of F = 0.77(3) and a coherence time of ${T}_{2}^{* }=2.60(8)$ ms. Our results show that a T centre in silicon photonics can realize a multi-qubit register with an optical interface for quantum communication.

Song, Hanbin [Lawrence Berkeley National Laborator↗

Environment-imposed selection rules for nuclear-spin conversion of H 2 in molecular crystals

Nuclear-spin conversion in molecular hydrogen is governed by strict symmetry rules that typically require magnetic fields or catalytic surfaces to break. Here we demonstrate that the intrinsic tensor composition of a non-magnetic molecular crystal field can impose and relax these rules without external fields. High-resolution infrared spectra of H 2 in crystalline CO 2 reveal large rank-2 (quadrupolar) crystal-field splittings of the 𝑚 sublevels, while nuclear-spin conversion occurs only through 𝛥𝑚 = 0 channels. Replacing CO 2 with polar N 2 O introduces rank-1 (dipole) components that partially open 𝛥⁢𝑚 ≠ 0 pathways, while incorporation of paramagnetic NO 2 fully lifts the restriction. Furthermore, these results establish a direct correspondence between crystal-field tensor rank and nuclear-spin dynamics, introducing a general symmetry-based framework for designing and controlling spin-isomer populations and quantum-state connectivity in molecular solids.

McLane, Nathan [University of Maryland, College Pa↗

Observation of nuclear-spin Seebeck effect

Thermoelectric effects have been applied to power generators and temperature sensors that convert waste heat into electricity. The effects, however, have been limited to electrons to occur, and inevitably disappear at low temperatures due to electronic entropy quenching. Here, we report thermoelectric generation caused by nuclear spins in a solid: nuclear-spin Seebeck effect. The sample is a magnetically ordered material MnCO 3 having a large nuclear spin ( I = 5/2) of 55 Mn nuclei and strong hyperfine coupling, with a Pt contact. In the system, we observe low-temperature thermoelectric signals down to 100 mK due to nuclear-spin excitation. Our theoretical calculation in which interfacial Korringa process is taken into consideration quantitatively reproduces the results. The nuclear thermoelectric effect demonstrated here offers a way for exploring thermoelectric science and technologies at ultralow temperatures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nuclear spin metrology with nitrogen vacancy center in diamond for axion dark matter detection

We present a method to directly detect the axion dark matter using nitrogen vacancy centers in diamonds. In particular, we use metrology leveraging the nuclear spin of nitrogen to detect axion-nucleus couplings. This is achieved through protocols designed for dark matter searches, which introduce a novel approach of quantum sensing techniques based on the nitrogen vacancy center. Although the coupling strength of the magnetic fields with nuclear spins is three orders of magnitude smaller than that with electron spins for conventional magnetometry, the axion interaction strength with nuclear spins is the same order of magnitude as that with electron spins. Furthermore, we can take advantage of the long coherence time by using the nuclear spins for the axion dark matter detection. Our method has the potential to be sensitive to a broad frequency range ≲ 100 Hz corresponding to the axion mass m a ≲ 4 × 10 − 13 eV . We present the detection limit of our method for both the axion-neutron and the axion-proton couplings and discuss its significance in comparison with other proposed ideas. We also show that the sensitivities of the NV center sensor to various spin species will open up new directions for constructing protocols that can mitigate magnetic noise effects. Published by the American Physical Society 2025

Chigusa, So (ORCID:0000000160054447)↗

Single nuclear spin detection and control in a van der Waals material

Optically active spin defects in solids are leading candidates for quantum sensing and quantum networking. Recently, single spin defects were discovered in hexagonal boron nitride (hBN), a layered van der Waals (vdW) material. Owing to its two-dimensional structure, hBN allows spin defects to be positioned closer to target samples than in three-dimensional crystals, making it ideal for atomic-scale quantum sensing, including nuclear magnetic resonance (NMR) of single molecules. However, the chemical structures of these defects remain unknown and detecting a single nuclear spin with a hBN spin defect has been elusive. Here we report the creation of single spin defects in hBN using 13 C ion implantation and the identification of three distinct defect types based on hyperfine interactions. We observed both S = 1/2 and S = 1 spin states within a single hBN spin defect. We demonstrated atomic-scale NMR and coherent control of individual nuclear spins in a vdW material, with a π-gate fidelity up to 99.75% at room temperature. By comparing experimental results with density functional theory (DFT) calculations, we propose chemical structures for these spin defects. Our work advances the understanding of single spin defects in hBN and provides a pathway to enhance quantum sensing using hBN spin defects with nuclear spins as quantum memories.

Quantum metrology↗

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↗

Model for nuclear spin product-state distributions of ultracold chemical reactions in magnetic fields

Based on a theoretical model where the nuclear spins remain unchanged during a collision, we provide an analytical and general expression for the nuclear spin state-to-state distribution of an ultracold diatom-diatom chemical reaction in a magnetic field, for given rotational transitions of the molecules. It simply requires knowledge of the field-dependent eigenfunctions of the molecular reactants and products of the chemical reaction. The final state-to-state distribution drastically changes with the magnetic field. When the distribution is summed over all the final products, a simplified expression is found where only the knowledge of the eigenfunctions of the molecular reactants is required. The present theoretical formalism has been successfully used to explain the magnetic field behavior of the product-state distribution in chemical reactions of ultracold KRb molecules [Hu et al., Nat. Chem. 13, 435 (2021)].

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Quantum optimal control of ten-level nuclear spin qudits in Sr 87

We study the ability to implement unitary maps on states of the I = 9 / 2 nuclear spin in Sr 87 , a d = 10 dimensional (qudecimal) Hilbert space, using quantum optimal control. Through a combination of nuclear spin resonance and a tensor ac Stark shift, by solely modulating the phase of a radio-frequency magnetic field, the system is quantum controllable. Alkaline-earth-metal atoms, such as Sr 87 , have a very favorable figure of merit for such control due to narrow intercombination lines and the large hyperfine splitting in the excited states. We numerically study the quantum speed limit, optimal parameters, and the fidelity of arbitrary state preparation and full SU(10) maps, including the presence of decoherence due to optical pumping induced by the light-shifting laser. We also study the use of robust control to mitigate some dephasing due to inhomogeneities in the light shift. We find that with an rf Rabi frequency of Ω rf and 0.5% inhomogeneity in the the light shift we can prepare an arbitrary Haar-random state in a time T = 4.5 π / Ω rf with average fidelity ( F ψ ) = 0.9992 , and an arbitrary Haar-random SU(10) map in a time T = 24 π / Ω rf with average fidelity ( F U ) = 0.9923 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Electrical Control of the Nuclear Spin States of Rare-Earth Adatoms

Rare-earth adatoms on surfaces have been studied for potential atomic-scale magnetic storage, quantum sensing, and quantum computing applications. Despite accumulating experimental efforts, a comprehensive description of the electronic configurations of the adatoms remains elusive. Here, we investigate two charge states and several electronic configurations, including 5d and 6s valence shells, for a Sm adatom on a MgO substrate using multiconfigurational ab initio methods, for the possibility of using the Sm nuclear spin levels as qubits. For the configurations in a neutral charge state, we find that the electronic ground state is a singlet, and thus the hyperfine interaction associated with the 147 Sm nucleus is absent, which may greatly enhance nuclear spin coherence time. The degeneracy of the nuclear levels is lifted by the nuclear quadrupole interaction. We show that the splitting of the nuclear levels can be controlled by a static electric field, and that Rabi oscillations between the nuclear levels can be induced by a time-dependent electric field. For the configurations in a singly charged state, electronic Kramers doublets are formed. The electronic configurations including an unpaired 6s orbital exhibit a strong hyperfine Stark effect due to a large Fermi contact contribution to the hyperfine interaction. In these configurations, electric-field-induced Rabi oscillations between the electronic-nuclear levels can occur at frequencies up to 3 orders of magnitude higher than those for the neutral charge state. The proposed system may be experimentally observed within scanning tunneling microscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Entanglement between a muon spin and $I>\frac{1}{2}$ nuclear spins

We report on the first example of quantum coherence between the spins of muons and quadrupolar nuclei. We observe this effect in vanadium intermetallic compounds which adopt the A15 crystal structure, and whose members include all technologically dominant superconductors. The entangled states are extremely sensitive to the local structural and electronic environments through the electric field gradient at the quadrupolar nuclei. This case-study demonstrates that positive muons can be used as a quantum sensing tool to probe also structural and charge related phenomena in materials, even in the absence of magnetic order.

Bonfà, Pietro↗

Nuclear spin assisted magnetic field angle sensing

Abstract Quantum sensing exploits the strong sensitivity of quantum systems to measure small external signals. The nitrogen-vacancy (NV) center in diamond is one of the most promising platforms for real-world quantum sensing applications, predominantly used as a magnetometer. However, its magnetic field sensitivity vanishes when a bias magnetic field acts perpendicular to the NV axis. Here, we introduce a different sensing strategy assisted by the nitrogen nuclear spin that uses the entanglement between the electron and nuclear spins to restore the magnetic field sensitivity. This, in turn, allows us to detect small changes in the magnetic field angle relative to the NV axis. Furthermore, based on the same underlying principle, we show that the NV coupling strength to magnetic noise, and hence its coherence time, exhibits a strong asymmetric angle dependence. This allows us to uncover the directional properties of the local magnetic environment and to realize maximal decoupling from anisotropic noise.

Physics↗

Dynamic Nuclear Spin Polarization Induced by the Edelstein Effect at Bi(111) Surfaces

Nuclear spin polarization induced by hyperfine interaction and mainly the Edelstein effect due to strong spin-orbit interaction, is investigated by quantum transport in Bi(111) thin film samples. The Bi(111) films are deposited on mica by van der Waals epitaxial growth. The Bi(111) films show micrometer-sized triangular islands with 0.39 nm step height, corresponding to the Bi(111) bilayer height. At low temperatures a high current density is applied to generate a nonequilibrium carrier spin polarization by mainly the Edelstein effect at the Bi(111) surface, which then induces dynamic nuclear polarization by hyperfine interaction. Here, comparative quantum magnetotransport antilocalization measurements indicate a suppression of antilocalization by the in-plane Overhauser field from the nuclear polarization and allow a quantification of the Overhauser field. Hence nuclear polarization was both achieved and quantified by a purely electronic transport-based approach.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

High field magnetometry with hyperpolarized nuclear spins

Abstract Quantum sensors have attracted broad interest in the quest towards sub-micronscale NMR spectroscopy. Such sensors predominantly operate at low magnetic fields. Instead, however, for high resolution spectroscopy, the high-field regime is naturally advantageous because it allows high absolute chemical shift discrimination. Here we demonstrate a high-field spin magnetometer constructed from an ensemble of hyperpolarized 13 C nuclear spins in diamond. They are initialized by Nitrogen Vacancy (NV) centers and protected along a transverse Bloch sphere axis for minute-long periods. When exposed to a time-varying (AC) magnetic field, they undergo secondary precessions that carry an imprint of its frequency and amplitude. For quantum sensing at 7T, we demonstrate detection bandwidth up to 7 kHz, a spectral resolution < 100mHz, and single-shot sensitivity of 410pT $$/\sqrt{{{{{{{{\rm{Hz}}}}}}}}}$$ / Hz . This work anticipates opportunities for microscale NMR chemical sensors constructed from hyperpolarized nanodiamonds and suggests applications of dynamic nuclear polarization (DNP) in quantum sensing.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗