Nuclear Spin Research Articles

Fine-structure changing collisions in 87Rb upon D2 excitation in the hyperfine Paschen-Back regime

Abstract We investigate fine structure changing collisions in 87Rb vapour upon D2 excitation in a thermal vapour at 75 ∘C; the atoms are placed in a 0.6 T axial magnetic field in order to gain access to the hyperfine Pashen-Back regime. Following optical excitation on the D2 line, the exothermic transfer 5P 3 / 2 → 5P 1 / 2 occurs as a consequence of buffer-gas collisions; the 87Rb subsequently emits a photon on the D1 transition. We employ single-photon counting apparatus to monitor the D1 fluorescence, with an etalon filter to provide high spectral resolution. By studying the D1 fluorescence when the D2 excitation laser is scanned, we see that during the collisional transfer process the m J ′ quantum number of the atom changes, but the nuclear spin projection quantum number, m I ′ , is conserved. A simple kinematic model incorporating a coefficient of restitution in the collision accounted for the change in velocity distribution of atoms undergoing collisions, and the resulting fluorescence lineshape. The experiment is conducted with a nominally ‘buffer-gas free’ vapour cell; our results show that fine structure changing collisions are important with such media, and point out possible implications for quantum-optics experiments in thermal vapours producing entangled photon pairs with the double ladder configuration, and solar physics magneto-optical filters.

Pursuing high-fidelity control of spin qubits in natural Si/SiGe quantum dot

Electron spins in silicon quantum dots are a promising platform for fault-tolerant quantum computing. Low-frequency noise, including nuclear spin fluctuations and charge noise, is a primary factor limiting gate fidelities. Suppressing this noise is crucial for high-fidelity qubit operations. Here, we report on a two-qubit quantum device in natural silicon with universal qubit control, designed to investigate the upper limits of gate fidelities in a non-purified Si/SiGe quantum dot device. By employing advanced device structures, qubit manipulation techniques, and optimization methods, we have achieved single-qubit gate fidelities exceeding 99% and a two-qubit controlled-Z (CZ) gate fidelity of 91%. Decoupled CZ gates are used to prepare Bell states with an average fidelity of 91%, typically exceeding previously reported values in natural silicon devices. These results underscore that even natural silicon has the potential to achieve high-fidelity gate operations, particularly with further optimization methods to suppress low-frequency noise.

Understanding the Spin of Metal Complexes from a Single-Molecule Perspective.

Compared with aggregate spin behavior, single-molecule spin behavior can be accurately understood, controlled, and applied at the level of basic building blocks. The potential of single-molecule electronic and nuclear spins for monitoring and control represents a beacon of promise for the advancement of molecular spin devices, which are fabricated by connecting a single molecule between two electrodes. Metal complexes, celebrated for their superior magnetic attributes, are widely used in the devices to explore spin effects. Moreover, single-molecule electrical techniques with high signal-to-noise ratio, temporal resolution, and reliability help to understand the spin characteristics. In this review, the focus is on the devices with metal complexes, especially single-molecule magnets, and systematically present experimental and theoretical state of the art of this field at the single-molecule level, including the fundamental concepts of the electronic and nuclear spin and their basic spin effects. Then, several experimental methods developed to regulate the spin characteristics of metal complexes at single-molecule level are introduced, as well as the corresponding intrinsic mechanisms. A brief discussion is provided on the comprehensive applications and the considerable challenges of single-molecule spin devices in detail, along with a prospect on the potential future directions of this field.

Effect of Exchange Dynamics on the NMR Relaxation of Water in Porous Silica.

The interaction of molecules, in particular, water, with solid interfaces has been studied by a multitude of methods, among them nuclear magnetic resonance spin relaxation. The frequency dependence of the relaxation times follows patterns that have been interpreted in terms of the molecular orientation and dynamics. Several different model approaches could successfully explain limiting cases of 1H relaxation dispersion in systems with rigid surfaces such as silica gel or glass, but none of them can reproduce the relaxation of both 1H and 2H nuclei, which differ in their respective relaxation mechanisms, dipolar vs quadrupolar. From detailed studies of the dynamics of hydration of water in biological materials, the importance of hydrogen and molecular exchange to the longitudinal relaxation time of T1 was demonstrated. In this work, exchange times of both H2O and D2O in hydrophilic silica gel are varied in a controlled fashion in a wide range using disodium hydrogen phosphate, and the effect of physical exchange on spin relaxation is quantified for the first time in such systems using the exchange-mediated reorientation model.

Effective M3Y-P2 interaction of study nuclear energy levels for 48Ti in fp shell model

In the fp-shell area of the 48Ti isotope (Z=22, N=26), examine the nuclear excitation energies using the nuclear shell model. The energy levels, total angular momentum, and parity of the nucleons outside the locked core 40Ca are calculated using the OXBASH algorithm for GX2, GX1A, KB3, and effective M3Y-P2 interactions. mixing together two orbital configurations. There was a good agreement between the model space vectors and energy levels and experimental data, but the agreement decreased when the realistic M3YP-2 interaction was used. The core polarisability effect has been used to accommodate the rejected space: core and higher organization via the L-S shell with an effective M3Y-P2 interaction. A comparison of the theoretical and experimental results has been conducted.

An architecture for two-qubit encoding in neutral ytterbium-171 atoms

We present an architecture for encoding two qubits within the optical “clock” transition and nuclear spin-1/2 degree of freedom of neutral ytterbium-171 atoms. Inspired by recent high-fidelity control of all pairs of states within this four-dimensional quotes space, we present a toolbox for intra-ququart (single-atom) one- and two-qubit gates, inter-ququart (two-atom) Rydberg-based two- and four-qubit gates, and quantum nondemolition (QND) readout. We then use this toolbox to demonstrate the advantages of the ququart encoding for entanglement distillation and quantum error correction which exhibit superior hardware efficiency and better performance in some cases since fewer two-atom operations are required. Finally, leveraging single-state QND readout in our ququart encoding, we present a unique approach to studying interactive circuits and to realizing a symmetry protected topological phase of a spin-1 chain with a shallow, constant-depth circuit.

A Practical Guide to Metal Ions Dynamic Nuclear Polarization in Materials Science

In this protocol we outline the practical aspects and methodology for performing metal ions-based dynamic nuclear polarization (MI-DNP), focusing on materials science applications. In MI-DNP polarization is transferred from unpaired electrons of paramagnetic metal ions to nearby nuclear spins, thereby increasing the sensitivity of NMR spectroscopy. The protocol encompasses detailed steps for i) selecting suitable metal ions dopants based on chemical, structural and electron paramagnetic resonance (EPR) considerations, ii) characterizing the concentration, homogeneity and EPR properties of the dopant and iii) performing the MI-DNP experiment itself, including optimization of the field position and reliable assessment of the DNP enhancement factors. By adhering to this protocol, the interested reader can implement the MI-DNP approach in an efficient way, facilitating spectroscopic studies of functional materials.

An instructional lab apparatus for quantum experiments with single nitrogen-vacancy centers in diamond

Hands-on experimental experience with quantum systems in the undergraduate physics curriculum provides students with a deeper understanding of quantum physics and equips them for the fast-growing quantum science industry. Here, we present an experimental apparatus for performing quantum experiments with single nitrogen-vacancy (NV) centers in diamond. This apparatus is capable of basic experiments such as single-qubit initialization, rotation, and measurement, as well as more advanced experiments investigating electron–nuclear spin interactions. We describe the basic physics of the NV center and give examples of potential experiments that can be performed with this apparatus. We also discuss the options and inherent trade-offs associated with the choice of diamond samples and hardware. The apparatus described here enables students to write their own experimental control and data analysis software from scratch, all within a single semester of a typical lab course, as well as to inspect the optical components and inner workings of the apparatus. We hope that this work can serve as a standalone resource for any institution that would like to integrate a quantum instructional lab into its undergraduate physics and engineering curriculum.

Predominantly electric storage ring with nuclear spin control capability

A predominantly electric E&m storage ring, with weak superimposed magnetic bending, is shown to be capable of storing two different particle type bunches, such as helion (h) and deuteron (d), or h and electron (e -), co-traveling with different velocities on the same central orbit. Rear-end collisions occurring periodically in a full acceptance particle detector/polarimeter, allow the (previously inaccessible) direct measurement of the spin dependence of nuclear transmutation for center of mass (CM) kinetic energies (KE) ranging from hundreds of keV up toward pion production thresholds. With the nuclear process occurring in a semi-relativistic moving frame, all initial and final state particles have convenient laboratory frame KEs in the tens to hundreds of MeV. The rear-end collisions occur as faster stored bunches pass through slower bunches. An inexpensive facility capable of meeting these requirements is described, with several nuclear channels as examples. Especially noteworthy are the e+/--induced weak interaction triton (t) β-decay processes, t + e + → h + ν and h + e - → t + ν. Experimental capability of measurement of the spin dependence of the induced triton case is emphasized. For cosmological nuclear physics, the experimental improvement will be produced by the storage ring's capability to investigate the spin dependence of nuclear transmutation processes at reduced kinetic energies compared to what can be obtained with fixed target geometry.

Dynamic Nuclear Polarization with Conductive Polymers

AbstractThe low sensitivity of liquid‐state nuclear magnetic resonance (NMR) can be overcome by hyperpolarizing nuclear spins by dissolution dynamic nuclear polarization (dDNP). It consists of transferring the near‐unity polarization of unpaired electron spins of stable radicals to the nuclear spins of interest at liquid helium temperatures, below 2 K, before melting the sample in view of hyperpolarized liquid‐state magnetic resonance experiments. Reaching such a temperature is challenging and requires complex instrumentation, which impedes the deployment of dDNP. Here, we propose organic conductive polymers such as polyaniline (PANI) as a new class of polarizing matrices and report 1H polarizations of up to 5 %. We also show that 13C spins of a host solution impregnated in porous conductive polymers can be hyperpolarized by relayed DNP. Such conductive polymers can be synthesized as chiral and display current induced spin selectivity leading to electron spin hyperpolarization close to unity without the need for low temperatures nor high magnetic fields. Our results show the feasibility of solid‐state DNP in conductive polymers that are known to exhibit chirality‐induced spin selectivity.

Ramsey interferometry of nuclear spins in diamond using stimulated Raman adiabatic passage

Abstract We report the first experimental demonstration of stimulated Raman adiabatic passage (STIRAP) in nuclear-spin transitions of 14N within nitrogenvacancy (NV) color centers in diamond. It is shown that the STIRAP technique suppresses the occupation of the intermediate state, which is a crucial factor for improvements in quantum sensing technology. Building on that advantage, we develop and implement a generalized version of the Ramsey interferometric scheme, employing half-STIRAP pulses to perform the necessary quantum-state manipulation with high fidelity. The enhanced robustness of the STIRAP-based Ramsey scheme to variations in the pulse parameters is experimentally demonstrated, showing good agreement with theoretical predictions. Our results pave the way for improving the long-term stability of diamond-based sensors, such as gyroscopes and frequency standards.

Accelerating T1 relaxation time measurements of noble gas using transverse low-frequency square-wave magnetic field modulation.

The longitudinal relaxation time (T1) of noble gas nuclear spins is a critical parameter for evaluating the performance of an atomic comagnetometer, significantly influencing the signal-to-noise ratio of the system. Traditional measurement techniques, such as the free induction decay method combined with the spin growth technique (FIDSG), are time-consuming for gases with extended T1 durations, such as 21Ne, and are prone to substantial environmental variability. Here, we propose the transverse low-frequency square-wave magnetic field modulation (LSMM) method for the rapid measurement of T1. The experiment indicates that the LSMM significantly condenses the measurement time to 19.2% of the original, thereby diminishing the robustness demands of the system. Although a minor discrepancy of up to 3 min (or 1.3%) exists between LSMM and FIDSG results, the LSMM method provides strong support for calibrating the performance of comagnetometer cells and conducting various nuclear spin polarization experiments, thereby improving efficiency and reducing energy loss.

Utilizing the multifrequency resonances of the electron spins in diamond nitrogen-vacancy centers under strong radio frequency driving for quantum sensing

Multifrequency resonances in the pulsed-optically detected magnetic resonance (ODMR) spectra of electron spins in ensemble nitrogen-vacancy (NV) centers in diamonds are investigated under strong radio frequency (RF) driving at a MHz frequency range and weak microwave driving at a GHz frequency range in a bias static magnetic field for quantum sensing applications. First, we demonstrate that the coherent destruction of tunneling, which leads to the disappearance of the main resonance peaks, can be utilized for precise calibration of the RF amplitude. Next, we clarify the condition for enhancing the sensitivity of a DC magnetic field under strong RF driving at the RF frequency that matches the split frequency due to the hyperfine interaction between 15N nuclear spins and the NV electron spins. Our findings indicate that strong RF driving increases the sensitivity of the DC magnetic field by enhancing the ODMR contrast and reducing the linewidth. The above results contribute to certifying the quantitative accuracy of RF imaging and enhancing the sensitivity of the DC magnetic field imaging using ensemble NV centers in diamonds.

Noise-Induced Quantum Synchronization and Entanglement in a Quantum Analogue of Huygens' Clock.

We propose a quantum analogue of the Huygens clock, where the phases of two spins synchronize through their interaction with a shared environment. This environment acts like the escapement mechanism in a mechanical clock, regulating the gear train and allowing discrete timing advances. In our model, the relative phases of the two spins synchronize via a mutually correlated environment. We demonstrate that several arguments can significantly reduce the cardinality of the allowed measurements for a system of qubits, thus simplifying the problem. We present a numerically efficient method to calculate the degree of quantumness in the correlations of the final density matrix, providing a tight upper bound for rank 3 and rank 4 density matrices. We suggest a potential realization of noise-induced synchronization between two nuclear spins coupled to a common ancilla undergoing dynamical decoupling.

Spin-bearing molecules as optically addressable platforms for quantum technologies

Abstract Efforts to harness quantum hardware relying on quantum mechanical principles have been steadily progressing. The search for novel material platforms that could spur the progress by providing new functionalities for solving the outstanding technological problems is however still active. Any physical property presenting two distinct energy states that can be found in a long-lived superposition state can serve as a quantum bit (qubit), the basic information processing unit in quantum technologies. Molecular systems that can feature electron and/or nuclear spin states together with optical transitions are one of the material platforms that can serve as optically addressable qubits. The attractiveness of molecular systems for quantum technologies relies on the fact that molecular structures of atomically defined nature can be obtained in endless diversity of chemical compositions. Crucially, by harnessing the molecular design protocols, the optical and spin (electronic and nuclear) properties of molecules can be tailored, aiding the design of optically addressable spin qubits and quantum sensors. In this contribution, we present a concise and collective discussion of optically addressable spin-bearing molecules – namely, organic molecules, transition metal (TM) and rare-earth ion (REI) complexes – and highlight recent results such as chemical tuning of optical and electron spin quantum coherence, optical spin initialization and readout, intramolecular quantum teleportation, optical coherent storage, and photonic-enhanced optical addressing. We envision that optically addressable spin-carrying molecules could become a scalable building block of quantum hardware for applications in the fields of quantum sensing, quantum communication and quantum computing.

SU(N) magnetism with ultracold molecules

Abstract Quantum systems with SU(N) symmetry are paradigmatic settings for quantum many-body physics. They have been studied for the insights they provide into complex materials and their ability to stabilize exotic ground states. Ultracold alkaline-earth atoms were predicted to exhibit SU(N) symmetry for N = 2I +1 = 1, 2, . . . , 10, where I is the nuclear spin. Subsequent experiments have revealed rich many-body physics. However, alkaline-earth atoms realize this symmetry only for fermions with repulsive interactions. In this paper, we predict that ultracold molecules shielded from destructive collisions with static electric fields or microwaves exhibit SU(N) symmetry, which holds because deviations of the s-wave scattering length from the spin-free values are only about 3% for CaF with static-field shielding and are estimated to be even smaller for bialkali molecules. They open the door to N as large as 32 for bosons and 36 for fermions. They offer important features unachievable with atoms, including bosonic systems and attractive interactions.

Muon spin force

Current discrepancy between the measurement and the prediction of the muon anomalous magnetic moment can be resolved in the presence of a long-range force created by ordinary atoms acting on the muon spin via axial-vector and/or pseudoscalar coupling, and requiring a tiny O(10−13 eV) spin energy splitting between muon state polarized in the vertical direction. We suggest that an extension of the muon spin resonance (μSR) experiments can provide a definitive test of this class of models. We also derive indirect constraints on the strength of the muon spin force by considering the muon-loop-induced interactions between nuclear spin and external directions. The limits on the muon spin force extracted from the comparison of Hg199/Hg201 and Xe129/Xe131 spin precession are strong for the pseudoscalar coupling but are significantly relaxed for the axial-vector one. These limits suffer from significant model uncertainties, poorly known proton/neutron spin content of these nuclei, and therefore do not exclude the possibility of a muon spin force relevant for the muon g−2. Published by the American Physical Society 2024

Quantum-enhanced Green's function Monte Carlo algorithm for excited states of the nuclear shell model

Quantum-enhanced Green's function Monte Carlo algorithm for excited states of the nuclear shell model

Highly Spin-Polarized Molecules via Collisional Microwave Pumping.

We propose a general technique to produce cold spin-polarized molecules in the electronic states of Σ symmetry, in which rotationally excited levels are first populated by coherent microwave excitation, and then allowed to spin flip and relax via collisional quenching, which populates a single final spin state. The steady-state spin polarization is maximized in the regime, where collisional slip-flipping transitions in the ground rotational manifold (N=0) are suppressed by a factor of ≥10 compared to those in the first rotationally excited manifold (N=1), as generally expected for Σ-state molecules at temperatures below the rotational spacing between the N=0 and N=1 manifolds. We theoretically demonstrate the high selectivity of the technique for ^{13}C^{16}O molecules immersed in a cold buffer gas of helium atoms, achieving a high degree (≥95%) of nuclear spin polarization at 1K.

Homogeneous Catalysts for Hydrogenative PHIP Used in Biomedical Applications

AbstractAt present, two competing hyperpolarization (HP) techniques, dissolution dynamic nuclear polarization (DNP) and parahydrogen (para‐H2) induced polarization (PHIP), can generate sufficiently high liquid state 13C signal enhancement for in vivo studies. PHIP utilizes the singlet spin state of para‐H2 to create non‐equilibrium spin populations. In hydrogenative PHIP, para‐H2 is irreversibly added to unsaturated precursors, typically in the presence of a homogeneous catalyst. The hydrogenation catalyst plays a crucial role in converting the singlet spin order of para‐H2 into detectable nuclear polarization. Currently, rhodium(I) bisphosphine complexes are the most widely employed catalysts for PHIP, capable of catalyzing the addition of para‐H2 to unsaturated precursors in organic solvents or aqueous media, depending on the ligand. Chiral catalysts enable the stereoselective production of hyperpolarized substrates. Ruthenium(II) piano stool complexes are capable of trans addition and are used to generate hyperpolarized fumarate. However, these catalysts systems are not optimal, and the greatest source of nuclear spin polarization loss is attributed to the mixing of singlet and triplet states of the protons derived from the para‐H2 during the hydrogenation process. Hence, future efforts should focus on enhancing the efficiency and kinetics of these catalysts.