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Noise spectroscopy elucidates the fundamental noise sources in spin systems, which is essential for developing spin qubits with long coherence times for quantum information processing, communication, and sensing. But noise spectroscopy typically relies on microwave coherent spin control to extract the noise spectrum, which becomes infeasible when there are high-frequency noise components stronger than the available microwave power. Here, we demonstrate an alternative all-optical approach to performing noise spectroscopy. Our approach utilises coherent Raman rotations of the spin state with controlled timing and phase to implement Carr-Purcell-Meiboom-Gill (CPMG) pulse sequences. Analysing the spin dynamics under these sequences enables us to extract the noise spectrum of a dense ensemble of nuclear spins interacting with a single spin in a quantum dot, which has thus far only been modelled theoretically. By providing large spectral bandwidths of over 100 MHz, our Raman-based approach could serve as an important tool to study spin dynamics and decoherence mechanisms for a broad range of solid-state spin qubits.

Quantum memories capable of storing and retrieving coherent information for extended times at room temperature would enable a host of new technologies. Electron and nuclear spin qubits using shallow neutral donors in semiconductors have been studied extensively but are limited to low temperatures ($\le$10 K); however, the nuclear spins of ionized donors have potential for high temperature operation. We use optical methods and dynamical decoupling to realize this potential for an ensemble of 31P donors in isotopically purified 28Si and observe a room temperature coherence time of over 39 minutes. We further show that a coherent spin superposition can be cycled from 4.2 K to room temperature and back, and report a cryogenic coherence time of 3 hours in the same system., 5 pages, 4 figures

Quantum state control is one of the most important concepts in advanced quantum technology, emerging quantum cybernetics and related fields. Molecular open shell entities can be a testing ground for implementing quantum control technology enabling us to manipulate molecular spin quantum bits (molecular spin qubits). In well-designed molecular spins consisting of unpaired electron and nuclear spins, the electrons and nuclear spins can be bus and client qubits, respectively. Full control of molecular spin qubits, in which client spins interact via hyperfine coupling, is a key issue for implementing quantum computers (QCs). In solid-state QCs, there are two approaches to the control of nuclear client qubits, namely, direct control of nuclear spins by radio-wave (RF) pulses and indirect control via hyperfine interactions by microwave pulses applied to electron spin qubits. Although the latter is less popular in the literature, the indirectness has advantage of greatly reducing unnecessary interactions between a qubit system and its environment. In this work, we investigate molecular spin optimization to find optimal experimental conditions which can afford to achieve the high fidelity of quantum gates by the indirect control scheme. In the present quantum systems, one electron is directly controlled by pulsed ESR techniques without manipulating individual hyperfine resonance, but the states of two nuclear client spins are indirectly steered via hyperfine interactions. Single crystals of potassium hydrogen maleate (KHM) radical and 13C-labeled malonyl radical are chosen as typical molecular spin qubits which exemplify the importance of the symmetry of hyperfine tensors and their collinear properties. We have found that both the non-collinearity of the principal axes of hyperfine coupling tensors and the non-distinguishability/non-equivalency between nuclear spins are key issues which extremely reduce the gate fidelity.

The spins, which are accumulated at a boundary of a nanomagnet due to the Spin Hall effect, induce a magnetic field, which tilts the nanomagnet magnetization out of its easy axis. Even though this magnetic field is relatively small (about 20 Gauss), it can reverse the magnetization of the nanomagnet if it is modulated in resonance with the magnetization precession and the conditions of the parametric resonance are met. Therefore, such magnetic field can be used to optimize the recording mechanism and to minimize the recording energy for MRAM. A high-precession measurement method of the spin-accumulation-induced magnetic field is developed. The magnetic field is measured in a FeCoB nanomagnet and its properties are studied., 5 pages, 6 figures

Annealing machines have been developed as non-von Neumann computers aimed at solving combinatorial optimization problems efficiently. To use annealing machines for solving combinatorial optimization problems, we have to represent the objective function and constraints by an Ising model, which is a theoretical model in statistical physics. Further, it is necessary to transform the Ising model according to the hardware limitations. In the transformation, the process of effectively reducing the bit-widths of coefficients in the Ising model has hardly been studied so far. Thus, when we consider the Ising model with a large bit-width, a naive method, which means right bit-shift, has to be applied. Since it is expected that obtaining highly accurate solutions is difficult by the naive method, it is necessary to construct a method for efficiently reducing the bit-width. This paper proposes methods for reducing the bit-widths of interaction and external magnetic field coefficients in the Ising model and proves that the reduction gives theoretically the same ground state of the original Ising model. The experimental evaluations also demonstrate the effectiveness of our proposed methods.

Summary The photomagnetic effect is known to be related only to transition metal atoms with empty orbitals and spin-state changes. In general, noble metals with high electron density cannot be used as photomagnetic materials because of the absence of spin polarization. However, here, we found that photomagnetic-chiral anisotropy (PM-ChA) was generated in chiral nanostructured Au films (CNAFs), and opposite photomagnetic fields (PMFs) were created in the antipodal CNAFs under unpolarized irradiation. The PM-ChA was speculated to arise from directional alignment of opposite spins polarized by the asymmetric spin-orbit coupling due to the opposite effective magnetic fields induced by electron motion in the antipodal helical structure. PM-ChA can be applied in enantiomeric quantification, probably because of the spin polarization coupling between CNAFs and enantiomers. PM-ChA of noble metals generated by directional spin control in helical nanostructures could provide new strategies in quantum technology and theories in magnetophysics.

We discovered new B-site-ordered double perovskites Ln2LiFeO6 (Ln = La, Nd, Sm, and Eu) with most likely unusually high valence Fe5+, which was stabilized by strong oxidizing high-pressure synthesis. Despite large antiferromagnetic interactions between Fe5+ spins in these compounds, the magnetic ordering is strongly suppressed due to the geometrical frustration of Fe5+ located in a face-centered cubic lattice. In addition, canted magnetic structures are stabilized only in those with Ln = Sm and Eu, which is most likely due to significant Dzyaloshinskii Moriya interaction caused by large monoclinic structural distortion. These results provide a deep understanding of the structure-property relationships in geometrically frustrated B-site-ordered double perovskites.

Transverse spin angular momentum of light is a key concept in recent nanophotonics to realize unidirectional light transport in waveguides by spin-momentum locking. Herein we theoretically propose subwavelength nanoparticle chain waveguides that efficiently sort optical spins with engineerable spin density distributions. By arranging high-refractive-index nanospheres of different sizes in a zigzag manner, directional optical spin propagation is realized. The origin of the efficient spin transport is revealed by analyzing the dispersion relation and spin angular momentum density distributions. In contrast to conventional waveguides, the proposed asymmetric waveguide can spatially separate up- and down-spins and locate one parity inside and the other outside the structure. Moreover, robustness against bending the waveguide and its application as an optical spin sorter are presented. Compared to previous reports on spatial engineering of local spins in photonic crystal waveguides, we achieved substantial miniaturization of the entire footprint down to subwavelength scale., 20 pages, 5 figures

Magnetic resonance force microscopy is becoming increasingly important for three-dimensional image reconstruction inside a sample with non-invasive measurements. In this study, a magnetic resonance force sensor with a vacuum-packaged magnetic cantilever was developed for the detection of free radicals in an atmospheric environment. A 1.5- $\mu \text{m}$ -thick silicon-based cantilever, which was mounted with a 25- $\mu \text{m}$ -diameter Nd-Fe-B magnet at the end of the cantilever, was hermetically packaged in a vacuum cavity using an anodic-bonding technique. The evaluation of the pressure dependence on the quality factor of the mechanical magnet-based cantilever revealed that the packaged-cavity pressure was approximately in the range of $7.3\,\,\times10$ 2– $1.0\,\,\times10$ 3 Pa after vacuum packaging. The corresponding detection sensitivity of the magnet-based cantilever sensor was calculated to be $1.1\,\,\times10$ -13 N/ $\sqrt {Hz} $ . Based on the magnetic force interaction, the magnetic field gradients were detected by mapping the variations in the resonant frequency and resonant amplitude of the magnetic cantilever. Finally, the magnetic resonance force, caused by the electron spin resonance in a standard radical of 1, 1-Diphenyl-2-picrylhydrazyl, was detected with a spin density of $\sim 1.5\,\,\times10$ 15 spins/cm3 in an atmospheric environment. The proposed vacuum-packaged magnet-based cantilever confirmed the high feasibility of magnetic resonance force detection within a non-hermetic environment.

Long-lived spin order-based approaches for magnetic resonance rely on the transition between two magnetic environments of different symmetry, one governed by the magnetic field of the spectrometer and the other where this strong magnetic field is inconsequential. Research on the excitation of magnetic-symmetry transitions in nuclear spins is a scientific field that debuted in Southampton in the years 2000. We advanced in this field carrying the baggage of pre-established directions in NMR spectroscopy. We propose to reveal in this text the part of discoveries that may have been obscured by our choice to only look at them through the experience of such pre-established directions, at the time. Focussing on potential applications, we may have insufficiently emphasised in the manuscripts the methodological developments that necessitated most scientific effort. Such methods developments foster most of the progress in NMR. Thus, we present the contributed mechanisms of translation between the symmetric and non-symmetric environments with respect to the main magnetic field B0, free of any utilitarian perspective. The concept of zero-quantum rotations in the starting blocks of long-lived state populations, magnetisation transfers between hyperpolarised heteronuclei and protons, and selective inversion for long-lived coherences are discussed, as well as hybrid 2D methods based on both insensitive nuclei excitation (“INEPT”) and long-lived spin order. We can see at this point that these magnetic wheels will take a longer time than we initially thought to set in motion new applications in studies of slow diffusion, angiography, or large-protein structure. However, these pulse sequences seed subsequent magnetic mechanisms that are sure to contribute to applications. For instance, some of the introduced coherence rotations were combined with classical pulse blocks to obtain 2D correlations between protons and heteronuclei. We hope the pulse sequence building blocks discussed herein open further perspectives for magnetic resonance experiments with long-lived spin order.

We consider a system of hierarchical interacting spins under dynamics of spin-flip type with a ferromagnetic mean field interaction, scaling with the hierarchical distance, coupled with a system of linearly interacting hierarchical diffusions of Ornstein-Uhlenbeck type. In particular, the diffusive variables enter in the spin-flip rates, effectively acting as dynamical magnetic fields. In absence of the diffusions, the spin-flip dynamics can be thought of as a modification of the Curie--Weiss model. We study the mean field and the two-level hierarchical model, in the latter case restricting to a subcritical regime, corresponding to high temperatures, obtaining macroscopic limits at different spatio-temporal scales and studying the phase transitions in the system. We also formulate a generalization of our results to the $k$-th level hierarchical case, for any $k$ finite, in the subcritical regime. We finally address the supercritical regime, in the zero-temperature limit, for the two-level hierarchical case, proceeding heuristically with the support of numerics., 44 pages, 17 figures

An investigation of spin and conformational dynamics in a series of symmetric Cu-Cu porphyrin dimer solutions is presented using electron paramagnetic resonance (EPR) spectroscopy. Previous spectral simulations focused on the isotropic exchange interaction (J avg) between the Cu centers. In this work, an additional line broadening parameter (J mod) is explored in detail via variable temperature X-band EPR in liquid solution for several different structures. The J mod phenomenon is due to fluctuations in the spin exchange interaction caused by conformational motion of the porphyrin planes. The J mod parameter scales with the inverse of the rotational barriers that determine the Boltzmann-weighted torsional angle distribution between neighboring porphyrin planes. Arrhenius plots allow for extraction of the activation energies for rotation, which are 5.77, 2.84, and 5.31 kJ/mol for ethyne-bridged (porphinato)copper(II)-(porphinato)copper(II), butadiyne-bridged (porphinato)copper(II)-(porphinato)copper(II), and ethyne-bridged (porphinato)copper(II)-(porphinato)zinc(II)-(porphinato)copper(II) complexes, respectively. DFT calculations of these torsional barriers match well with the experimental results. This is the first report of a J mod analysis within a highly anisotropic hyperfine field and demonstrates the utility of the theory for extraction of dynamic information.

Many birds are endowed with a visual magnetic sense that may exploit magnetosensitive radical recombination processes in the protein cryptochrome. In this widely accepted but unproven model, geomagnetic sensitivity is suggested to arise from variations in the recombination rate of a pair of radicals, whose unpaired electron spins undergo coherent singlet-triplet interconversion in the geomagnetic field by coupling to nuclear spins via hyperfine interactions. However, simulations of this conventional radical pair mechanism (RPM) predicted only tiny magnetosensitivities for realistic conditions because the RPM's directional sensitivity is strongly suppressed by the intrinsic electron-electron dipolar (EED) interactions, casting doubt on its viability as a magnetic sensor. We show how this RPM-suppression problem is overcome in a three-radical system in which a third "scavenger" radical reacts with one member of the primary pair. We use this finding to predict substantial magnetic field effects that exceed those of the RPM in the presence of EED interactions in animal cryptochromes.

We perform magnetic susceptibility and magnetic torque measurements on the organic $\kappa$-(BEDT-TTF)$_2$Hg(SCN)$_2$Br, which is recently suggested to host an exotic quantum dipole-liquid in its low-temperature insulating phase. Below the metal-insulator transition temperature, the magnetic susceptibility follows a Curie-Weiss law with a positive Curie-Weiss temperature, and a particular $M\propto \sqrt{H}$ curve is observed. The emergent ferromagnetically interacting spins amount to about 1/6 of the full spin moment of localized charges. Taking account of the possible inhomogeneous quasi-charge-order that forms a dipole-liquid, we construct a model of antiferromagnetically interacting spin chains in two adjacent charge-ordered domains, which are coupled via fluctuating charges on a Mott-dimer at the boundary. We find that the charge fluctuations can draw a weak ferromagnetic moment out of the spin singlet domains., Comment: 9 pages, 5 figures, Supplementary Material attached

Disordered exchange pair-distribution function is considered for up and down spins that are different from both cases in the high- and low-density limits. The coupling parameter r s and spin-polarization parameter ξ change in calculations. Disordered exchange pair-distribution function decreases with increasing coupling parameters. The exchange pair-distribution function in disordered two-dimensional (2D) electron gas depends on the density parameter, spin-polarization parameter, and spatial coordinates. Results show that the increase of the coupling parameter can be nearly compensated by increased disorders.

Molecular electronic spins are good candidates as qubits since they are characterized by a large tunability of their electronic and magnetic properties through a rational chemical design. Coordination compounds of light transition metals are promising systems for spin-based quantum information technologies, thanks to their long spin coherence times up to room temperature. Our work aims at presenting an in-depth study on how the spin-phonon coupling in vanadyl-acetylacetonate, [VO(acac)2], can change as a function of temperature using terahertz time-domain spectroscopy and density functional theory (DFT) calculations. Powder THz spectra were recorded between 10 and 300 K. The temperature dependence of vibrational frequencies was then accounted for in the periodic DFT calculations using unit-cell parameters measured at two different temperatures and the optimized ones, as usually reported in the literature. In this way, it was possible to calculate the observed THz anharmonic frequency shift with high accuracy. The overall differences in the spin-phonon coupling magnitudes as a function of temperature were also highlighted showing that the computed trends have to be ascribed to the anisotropic variation of cell parameters.

We study complex integrable systems on quiver varieties associated with the cyclic quiver, and prove their superintegrability by explicitly constructing first integrals. We interpret them as rational Calogero-Moser systems endowed with internal degrees of freedom called spins. They encompass the usual systems in type $A_{n-1}$ and $B_n$, as well as generalisations introduced by Chalykh and Silantyev in connection with the multicomponent KP hierarchy. We also prove that superintegrability is preserved when a harmonic oscillator potential is added., v2: 15 pages, accepted in Nonlinearity

A first example of an sp2 carbon-conjugated three-dimensional (3D) covalent organic framework (COF) (BUCT-COF-4) is synthesized via the Knoevenagel condensation of the saddle-shaped aldehyde-substituted cyclooctatetrathiophene and 1,4-phenylenediacetonitrile. Ascribed to the extended π-conjugation and long-range ordered structures, BUCT-COF-4 displays high Hall electron mobility of 1.97 cm2 V-1 s-1 at room temperature. After it is doped with iodine, the material not only exhibits an enhanced electron mobility up to 2.62 cm2 V-1 s-1 in ambient air but also presents an unexpected metal-free ferromagnetic phase transition arising from the formation of aligned spins unidirectional across the whole sp2 carbon-conjugated 3D framework. This is the first report of a ferromagnetic phenomenon in 3D COF materials, which would broaden promising applications and open a new frontier in COF materials.

The transverse relaxation time of the spin-exchange optical pumped noble gas nuclei is a fundamental parameter to evaluate the performance of a nuclear magnetic resonance (NMR) rotation sensor. In practical tests and applications, measuring the transverse relaxation time in real-time is challenging. Due to the conflict with feedback loops, the traditional methods are unsuitable for real-time measurement. To address this limitation, this paper proposes a real-time method based on parameter identification to measure the transverse relaxation time. In the proposed method, a step signal is added to the oscillation magnetic field to excite nuclear spins, and the phase response generated is collected for identification. An NMR rotation sensor prototype is developed for the proof of concept. The experimental results verify the effectiveness and the feasibility of the proposed method.

In recent years, several magnetic Mott insulators with strong spin-orbit coupling were suggested to be proximate to the Kitaev quantum spin liquid, whose one of the most exciting features is the fractionalization of spin excitations into itinerant Majorana fermions and static Z2 fluxes. Unfortunately, the ground states of these systems cannot be easily captured by experiment, remaining featureless to conventional local probes. Here, we propose to study the signatures of fractionalized excitations by exploiting their coupling to the lattice vibrations, dubbed magnetoelastic coupling, which arises from the fact that the interaction between spins depends on the relative distance between them. We argue that the magnetoelastic coupling can lead to the distinct modification of the phonon dynamics, which can be observed by measuring renormalized phonon spectrum, the sound attenuation, and the phonon Hall viscosity. This makes the phonon dynamics a promising tool for the characterization and identification of quantum spin liquid phases. In this work, we focus on the magnetoelastic effects in the three-dimensional Kitaev model realized on the hyperhoneycomb lattice. The hyperhoneycomb Kitaev spin liquid is particularly interesting since the strong Kitaev interaction was observed in the Kitaev magnet β-Li2IrO3, for which the spin-orbit entangled Jeff = 1/2 moments of iridium ions form precisely the hyperhoneycomb lattice.

A data-driven framework is presented for building magneto-elastic machine-learning interatomic potentials (ML-IAPs) for large-scale spin-lattice dynamics simulations. The magneto-elastic ML-IAPs are constructed by coupling a collective atomic spin model with an ML-IAP. Together they represent a potential energy surface from which the mechanical forces on the atoms and the precession dynamics of the atomic spins are computed. Both the atomic spin model and the ML-IAP are parametrized on data from first-principles calculations. We demonstrate the efficacy of our data-driven framework across magneto-structural phase transitions by generating a magneto-elastic ML-IAP for α-iron. The combined potential energy surface yields excellent agreement with first-principles magneto-elastic calculations and quantitative predictions of diverse materials properties including bulk modulus, magnetization, and specific heat across the ferromagnetic–paramagnetic phase transition.

Aromatic side chains are attractive probes of protein dynamic, since they are often key residues in enzyme active sites and protein binding sites. Dynamic processes on microsecond to millisecond timescales can be studied by relaxation dispersion experiments that attenuate conformational exchange contributions to the transverse relaxation rate by varying the refocusing frequency of applied radio-frequency fields implemented as either CPMG pulse trains or continuous spin-lock periods. Here we present an aromatic 1H R1ρ relaxation dispersion experiment enabling studies of two to three times faster exchange processes than achievable by existing experiments for aromatic side chains. We show that site-specific isotope labeling schemes generating isolated 1H–13C spin pairs with vicinal 2H–12C moieties are necessary to avoid anomalous relaxation dispersion profiles caused by Hartmann–Hahn matching due to the 3JHH couplings and limited chemical shift differences among 1H spins in phenylalanine, tyrosine and the six-ring moiety of tryptophan. This labeling pattern is sufficient in that remote protons do not cause additional complications. We validated the approach by measuring ring-flip kinetics in the small protein GB1. The determined rate constants, kflip, agree well with previous results from 13C R1ρ relaxation dispersion experiments, and yield 1H chemical shift differences between the two sides of the ring in good agreement with values measured under slow-exchange conditions. The aromatic1H R1ρ relaxation dispersion experiment in combination with the site-selective 1H–13C/2H–12C labeling scheme enable measurement of exchange rates up to kex = 2kflip = 80,000 s–1, and serve as a useful complement to previously developed 13C-based methods.

We consider the case that four spin-3 atoms are confined in an optical trap. The temperature is so low that the spatial degrees of freedom have been frozen. Exact numerical and analytical solutions for the spin-states have been both obtained. Two kinds of phase-diagrams for the ground states (g.s.) have been plotted. In general, the eigen-states with the total-spin S (a good quantum number) can be expanded in terms of a few basis-states $$f_{S,i}$$ f S , i . Let $$P_{f_{S,i}}^{\lambda }$$ P f S , i λ be the probability of a pair of spins coupled to $$\lambda =0, 2, 4$$ λ = 0 , 2 , 4 , and 6 in the $$f_{S,i}$$ f S , i state. Obviously, when the strength $$g_{\lambda }$$ g λ of the $$\lambda $$ λ -channel is more negative, the basis-state with the largest $$P_{f_{S,i}}^{\lambda }$$ P f S , i λ would be more preferred by the g.s.. When two strengths are more negative, the two basis-states with the two largest probabilities would be more important components. Thus, based on the probabilities, the spin-structures (described via the basis-states) can be understood. Furthermore, all the details in the phase-diagrams, say, the critical points of transition, can also be explained. Note that, for $$f_{S,i}$$ f S , i , $$P_{f_{S,i}}^{\lambda }$$ P f S , i λ is completely determined by symmetry. Thus, symmetry plays a very important role in determining the spin-structure of the g.s..