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Static and dynamic magnetic properties of the spiin-$\frac{5}{2}$triangle lattice antiferromagnet Na 3 Fe(PO 4 ) 2 studied by 31 P NMR

We report 31 P nuclear magnetic resonance (NMR) measurements have been carried out to investigate the magnetic properties and spin dynamics of Fe 3+ (S = 5/2) spins in the two-dimensional triangular lattice (TL) compound Na 3 Fe(PO 4 ) 2 . The temperature (T) dependence of nuclear spin-lattice relaxation rates (1/T 1 ) shows a clear peak around Néel temperature, T N = 10.9 K, corresponding to an antiferromagnetic (AFM) transition. From the temperature dependence of NMR shift (K) above T N , an exchange coupling between Fe 3+ spins was estimated to be J/k B ≃ 1.9 K using the spin-5/2 Heisenberg isotropic-TL model. The temperature dependence of 1/T 1 T divided by the magnetic susceptibility (χ), 1/T 1 T χ , above T N proves the AFM nature of spin fluctuations below ~50 K in the paramagnetic state. In the magnetically ordered state below T N , the characteristic rectangular shape of the NMR spectra is observed, indicative of a commensurate AFM state in its ground state. The strong temperature dependence of 1/T 1 in the AFM state is well explained by the two-magnon (Raman) process of the spin waves in a 3D antiferromagnet with a spin-anisotropy energy gap of 5.7 K. The temperature dependence of sublattice magnetization is also well reproduced by the spin waves. Those results indicate that the magnetically ordered state of Na 3 Fe(PO 4 ) 2 is a conventional 3D AFM state, and no obvious spin frustration effects were detected in its ground state

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Slow spin dynamics in the hyperhoneycomb lattice [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 revealed by H 1 NMR studies

We report the results of magnetic susceptibility χ and H 1 nuclear magnetic resonance (NMR) measurements on a three-dimensional hyperhoneycomb lattice compound [ ( C 2 H 5 ) 3 NH ] 2 Cu 2 ( C 2 O 4 ) 3 (CCCO). The average value of the antiferromagnetic (AFM) exchange coupling between the Cu 2 + ( S = 1 / 2 ) spins was determined to be J ~ 50 K from the χ measurements. No long-range magnetic ordering has been observed down to T = 50 mK, although NMR lines become slightly broader at low temperatures below 1 K. The broadening of the NMR spectrum observed below 1 K reveals that the Cu spin moments remain at this temperature, suggesting a non-spin-singlet ground state. The temperature and magnetic field dependence of 1 / T 1 at temperatures above 20 K is well explained by paramagnetic thermal spin fluctuations where the fluctuation frequency of Cu 2 + spins is higher than the NMR frequency of the order of megahertz. However, a clear signature of the slowing down of the Cu 2 + spin fluctuations was observed at low temperatures where 1 / T 1 shows a thermally activated behavior. The magnetic field dependence of the magnitude of the spin excitation gap suggests that the magnetic behaviors of CCCO are characterized as an AFM chain at low temperatures.

1-dimensional systems↗

Horizontal 1 K refrigerator with novel loading mechanism for polarized solid targets

We describe a helium evaporation refrigerator used to cool dynamically polarized proton and deuteron targets for electron-scattering experiments using the CEBAF Large Acceptance Spectrometer CLAS12 at Jefferson Lab. The geometry of the CLAS12 detector systems places severe design and construction constraints on the refrigerator and its ancillary equipment, resulting in a horizontal cryostat with a length of 4 m. The 16 cm 3 target samples, consisting of frozen ammonia (NH 3 or ND 3 ), are loaded at the upstream end of the cryostat and moved to the beam-interaction region using a novel transport mechanism. At this location they are cooled with superfluid helium and polarized via dynamic nuclear polarization at 1 K and 5 T. In this manner samples can be replaced and cooled to 1 K in about 30 minutes without disturbing any elements of the electron beam line or particle detection system. In conclusion, we estimate that this method saved 18 days of valuable beam time over the course of a recent, 88-day long experiment.

Evaporation refrigerator↗

Multimodal spectroscopy of order parameter distributions

We present a multimodal spectroscopic paradigm that enables independent measurement of charge and spin degrees of freedom (DOF) in strongly correlated materials. This spin-based technique probes symmetry-specific Hamiltonian parameters by analyzing how the time delay between applied pulses (τ) affects the response. We demonstrate ways in which charge DOF that couple through the quadrupolar interaction (inversion symmetric) can be independently measured even in the presence of large magnetic noise (inversion asymmetric). The method quantifies both the strength of the interactions and their distribution (noise). We provide protocols to directly and independently measure the distribution of interaction strengths, even when the average value of the interaction is zero. By independently measuring distributions of different forms of disorder, this methodology can elucidate which microscopic symmetry drives a phase transition. Here, we discuss potential applications to study complex phase transitions in strongly interacting quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impact of Irradiation-induced Lattice Defects and Dopants on Thermal Transport in Oxide Nuclear Fuels

Advanced nuclear reactor concepts aim to use fuels that must withstand unprecedented temperature and radiation extremes. In these fuels, thermal energy transport under irradiation is directly related to fuel longevity, reactor safety, and is arguably one of the most important performance metrics. Here we provide a comprehensive, first-principles-informed treatment of phonon mediated thermal transport in a defect-bearing actinide oxide with direct comparison to experimental measurements. Pristine and proton irradiated thorium dioxide was chosen as a model system to treat the complexity of thermal transport in the presence of lattice defects. A thermal transport model is implemented using the linearized Boltzmann transport equation (LBTE) with input from first principles calculations and defect evolution models. The output of the LBTE is compared directly to mesoscopic measurements of thermal conductivity on length scales commensurate with defect accumulation. Parametric measurements of conductivity with irradiation dose and temperature reveal a monotonic decrease in conductivity with irradiation dose, in the range of 0.001 dpa to 0.1 dpa. Besides radiation-induced defects, doping the thorium dioxide crystal with small quantities of uranium atoms also results in a drastic reduction in thermal conductivity. Temperature-dependent measurements of thermal conductivity in uranium-doped thorium dioxide single crystals suggests a resonant scattering mechanism is responsible for the observed reduction. This comprehensive, atomistic- to meso-scale treatment provides the necessary basis to investigate thermal transport under irradiation in more complex systems that exhibit strong electron correlation. This is a poster presentation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nodeless superconductivity in the noncentrosymmetric compound ThIrSi

The superconductor ThIrSi, with Tc=6.5K, is expected to show unusual features in view of its noncentrosymmetric structure and the presence of heavy elements featuring a sizable spin-orbit coupling. Here, we report a comprehensive study of its electronic properties by means of magnetization, muon-spin rotation and relaxation (μ⁢SR) and nuclear magnetic resonance (NMR) measurements. Both the superfluid density ρ sc ⁡(T) (determined via transverse-field μ⁢SR) and the spin-lattice relaxation rate T–1 1⁡(T) (determined via NMR) suggest a nodeless superconductivity. Furthermore, the absence of spontaneous magnetic fields below T c , as evinced from zero-field μ⁢SR measurements, indicates a preserved time-reversal symmetry in the superconducting state of ThIrSi. Finally, temperature-dependent upper critical fields as well as field-dependent superconducting muon-spin relaxations suggest the presence of multiple superconducting gaps in ThIrSi.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Accelerated thermal property mapping of TRISO advanced nuclear fuel

TRistructural ISOtropic (TRISO) fuel is a leading-edge nuclear fuel form representing a departure from the more traditional nuclear fuel forms utilized in the reactor fleet of today. Rather than a monolithic fuel pellet of uranium dioxide, integral fuel forms containing TRISO fuel are composed of thousands of microencapsulated uranium-bearing fuel kernels and individually coated with multiple layers of pyrolytic carbon and silicon carbide. These multilayered ceramic coatings serve as an environmental barrier to ensure radioactive and chemically reactive fission products are contained within the reactor fuel elements, but also participate in the transfer of heat generated in the nuclear fuel to the coolant – the primary purpose of a nuclear reactor. Since traditional thermal property measurement techniques, such as laser flash analysis, would be unable to resolve the thermal properties of the individual TRISO coating layers, a simplified frequency-domain thermoreflectance technique has been developed to rapidly map the thermal properties of TRISO particles. Using this technique, the thermal properties of TRISO particles have been mapped from room temperature up to 1000 °C to examine the spatial variation and temperature-dependency of the thermal properties within each layer. Additionally, spatial-domain thermoreflectance was used to examine the anisotropy of the thermal properties for each layer at different locations within a single TRISO particle, and across multiple TRISO particles to assess the intra- and inter-particle uniformity of thermal properties, respectively. To elucidate the underlying causes for the measured variations in thermal properties, scanning electron microscopy and Raman spectroscopy were used to examine variations in microstructure and chemical bonding within the different coating layers. Results from this work are then compared with previous examinations of TRISO fuel particles and microstructurally driven mechanisms for the variations in the measured thermal properties of the different carbonaceous layers are discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Inhomogeneous magnetic ordered state and evolution of magnetic fluctuations in Sr⁢(Co 1–x ⁢Ni x ) 2 ⁢P 2 revealed by 31 P NMR

SrCo 2 ⁢P 2 with a tetragonal structure is known to be a Stoner-enhanced Pauli paramagnetic metal being nearly ferromagnetic. Recently J. Schmidt et al. [Phys. Rev. B 108, 174415 (2023)] reported that a ferromagnetic ordered state is actually induced by a small Ni substitution for Co of x = 0.02 in Sr⁢(Co 1–x ⁢Ni x ) 2 ⁢P 2 where an antiferromagnetic ordered phase also appears by further Ni substitution with x = 0.06–0.35. Here, in this work, using nuclear magnetic resonance (NMR) measurements on 31 P nuclei, we have investigated how the magnetic properties change by the Ni substitution in Sr⁢(Co 1–x ⁢Ni x ) 2 ⁢P 2 from a microscopic point of view, especially focusing on the evolution of magnetic fluctuations with the Ni substitution and the characterization of the magnetically ordered states. The temperature dependencies of the 31 P spin-lattice relaxation rate divided by temperature (1/T 1 ⁢T) and Knight shift (K) for SrCo 2 ⁢P 2 are reasonably explained by a model where a double-peak structure for the density of states near the Fermi energy is assumed. Based on a Korringa ratio analysis using the T 1 and K data, ferromagnetic spin fluctuations are found to dominate in the ferromagnetic Sr⁢(Co 1–x ⁢Ni x ) 2 ⁢P 2 as well as the antiferromagnets where no clear antiferromagnetic fluctuations are observed. We also found the distribution of the ordered Co moments in the magnetically ordered states from the analysis of the 31 P-NMR spectra exhibiting a characteristic rectangular-like shape.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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↗

Experimental confirmation of first-principles thermal conductivity in Zirconium-doped ThO 2

The degradation of thermal conductivity in advanced nuclear fuels due to the accumulation of fission products and irradiation-induced defects is inevitable, and must be considered as part of safety and efficiency analyses of nuclear reactors. Here, this study examines the thermal conductivity of a zirconium-doped ThO 2 crystal, synthesized via the hydrothermal method using a spatial domain thermoreflectance technique. Zirconium is one of the soluble fission products in oxide fuels that can effectively scatter heat-carrying phonons in the crystalline lattice of fuel. Thus, thermal property measurements of zirconium-doped ThO 2 single crystals provide insights into the effects of substitutional zirconium doping, isolated from extrinsic factors such as grain boundary scattering. The experimental results are compared with first-principles calculations of the lattice thermal conductivity of ThO 2 , employing an iterative solution of the Peierls-Boltzmann transport equation. Additionally, the non-perturbative Green's function methodology is utilized to compute phonon-point defect scattering rates, accounting for local distortions around point defects, including mass difference changes, interatomic force constants, and structural relaxation. The congruence between the predicted results from first-principles calculations and the measured temperature-dependent thermal conductivity validates the computational methodology. Furthermore, the methodologies employed in this study enable systematic investigations of thermal conductivity reduction by fission products, potentially leading to the development of more accurate fuel performance codes.

36 - MATERIALS SCIENCE↗

The phase diagram of ultra quantum liquids

In this paper, we discuss the dependence of the phase diagram of a hypothetical isotope of helium with nuclear mass less than 4 atomic mass units. We argue that with decreasing nucleus mass, the temperature of the superfluid phase transition (about 2.2 K in real 4 He) increases, while that of the liquid-gas critical point (about 5.2 K in real 4 He) decreases. We discuss various scenarios that may occur when the two temperatures approach each other and the order parameters of the superfluid and the liquid-gas phase transitions interact with each other. The simplest scenario, in which both order parameters become critical at particular values of the nuclear mass, temperature, and pressure, can be ruled out through on an analysis of the Landau theory. We argue that in the most likely scenario, as the nuclear mass decreases, first, a tricritical point appears on the line separating the superfluid and the normal fluid phase, then the critical point disappears under the first-order part of superfluid phase transition line, and in the end the tricritical point disappears. The last change in the phase diagram occurs when the two-body scattering length crosses zero, which corresponds to the nuclear mass of about 1.55 u. We develop a quantitative theory that allows one to determine the phase diagram in the vicinity of this point. Lastly, we discuss several ways to physically realize such liquids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Incommensurate and commensurate antiferromagnetic states in Ca Mn 2 As 2 and Sr Mn 2 As 2 revealed by As 75 NMR

Here, we carried out 75 As nuclear magnetic resonance (NMR) measurements on the trigonal CaMn 2 As 2 and SrMn 2 As 2 insulators exhibiting antiferromagnetic (AFM) ordered states below Néel temperatures T N = 62 and 120 K, respectively. In the paramagnetic state above T N , typical quadrupolar-split 75 As NMR spectra were observed for both systems. The 75 As quadrupolar frequency ν Q for CaMn 2 As 2 decreases with decreasing temperature, while ν Q for SrMn 2 As 2 increases, showing an opposite temperature dependence. In the AFM state, the relatively sharp and distinct 75 As NMR lines were observed in SrMn 2 As 2 and the NMR spectra were shifted to lower fields for both magnetic fields H ∥ c axis and H ∥ a b plane, suggesting that the internal fields B int at the As site produced by the Mn ordered moments are nearly perpendicular to the external magnetic field direction. No obvious distribution of B int was observed in SrMn 2 As 2 , which clearly indicates a commensurate AFM state. In sharp contrast to SrMn 2 As 2 , broad and complex NMR spectra were observed in CaMn 2 As 2 in the AFM state, which clearly shows a distribution of B int at the As site, indicating an incommensurate state. From the analysis of the characteristic shape of the observed spectra, the AFM state of CaMn 2 As 2 was determined to be a two-dimensional incommensurate state where Mn ordered moments are aligned in the ab plane. A possible origin for the different AFM states in the systems was discussed. Both CaMn 2 As 2 and SrMn 2 As 2 show very large anisotropy in the nuclear spin-lattice relaxation rate 1/T 1 in the paramagnetic state. 1/T 1 for H ∥ ab is much larger than that for H ∥ c, indicating strong anisotropic AFM spin fluctuations in both compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Microscopic characterization of the magnetic properties of the itinerant antiferromagnet La 2 Ni 7 by La 139 NMR/NQR measurements

In this study, 139 La nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements have been performed to investigate the magnetic properties of the itinerant magnet La 2 Ni 7 , which shows a series of antiferromagnetic (AFM) phase transitions at T N1 = 61 K, T N2 = 56 K, and T N3 = 42 K under zero magnetic field. Two distinct La NMR signals were observed due to the two crystallographically inequivalent La sites in La 2 Ni 7 (La1 and La2 in the La 2 Ni 4 and the LaNi 5 subunits of the La 2 Ni 7 unit cell, respectively). From the 139 La NQR spectrum in the AFM state below T N3 , the AFM state was revealed to be a commensurate state where Ni-ordered moments align along the crystalline c axis. Owing to the two different La sites, we were able to estimate the average values of the Ni-ordered moments (0.09 – 0.10 μB / Ni and 0.17 μB / Ni around La1 and La2, respectively) from 139 La NMR spectrum measurements in the AFM state below T N3 , suggesting a nonuniform distribution of the Ni-ordered moments in the AFM state. In contrast, a more uniform distribution of the Ni-ordered moments in the saturated paramagnetic state induced by the application of high magnetic fields is observed. The temperature dependence of the sublattice magnetization measured by the internal magnetic induction at the La2 site in the AFM state was reproduced by a local-moment model better than the self-consistent renormalization (SCR) theory for weak itinerant antiferromagnets. Given the small Ni-ordered moments in the magnetically ordered state, our results suggest that La 2 Ni 7 has characteristics of both itinerant nature and localized nature in its magnetism. With this in mind, it is noteworthy that the temperature dependence of nuclear spin-relaxation rates (1/T 1 ) in the paramagnetic state above T N1 measured at zero magnetic field can be explained qualitatively by both the SCR theory and the local-moment model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Probing ab initio emergence of nuclear rotation

Structural phenomena in nuclei, from shell structure and clustering to superfluidity and collective rotations and vibrations, reflect emergent degrees of freedom. Ab initio theory describes nuclei directly from a fully microscopic formulation. We can therefore look to ab initio theory as a means of exploring the emergence of effective degrees of freedom in nuclei. For the illustrative case of emergent rotational bands in the $Be$ isotopes, we establish an understanding of the underlying oscillator space and angular momentum (orbital and spin) structure. We consider no-core configuration interaction (NCCI) calculations for 7, 9, 11 Be with the Daejeon16 internucleon interaction. Although shell model or rotational degrees of freedom are not assumed in the ab initio theory, the NCCI results are suggestive of the emergence of effective shell model degrees of freedom (0$\hbar$ω and 2$\hbar$ω excitations) and LS-scheme rotational degrees of freedom, consistent with an Elliott–Wilsdon SU(3) description. Finally, these results provide some basic insight into the connection between emergent effective collective rotational and shell model degrees of freedom in these light nuclei and the underlying ab initio microscopic description.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Analysis of radially resolved thermal conductivity in high burnup mixed oxide fuel and comparison to thermal conductivity correlations implemented in fuel performance codes

The thermal diffusivity and thermal conductivity of high burnup (19 % FIMA) mixed oxide (U, Pu)O 2 nuclear fuel has been measured along the radial direction using a thermoreflectance-based method. Measured thermal conductivity exhibits a notable radial variation consistent with the expectations that a large temperature gradient across the annular fuel pellet leads to a heterogeneous microstructure. A common fuel performance model of thermal conductivity, the Lucuta-Inoue model, is used to analyze the measured thermal conductivity profile. Further, this model adequately captures the radial dependence of thermal conductivity except in the periphery. The analysis suggests that the characteristic radial shape of the thermal conductivity profile follows the burnup profile within the fuel pin. In the periphery, the high burnup structure is formed and the conductivity model, not capturing this effect, likely overestimates the thermal conductivity.

36 MATERIALS SCIENCE↗

A combined theoretical-experimental investigation of thermal transport in low-dose irradiated thorium dioxide

During reactor operation, nuclear fuels are subject to extreme temperature and irradiation conditions which can significantly degrade the fuel's thermal transport properties. The reduction in thermal conductivity of the fuel as a result of irradiation-induced lattice defects is arguably the most important fuel performance metric in regard to reactor efficiency and safety. Because thorium dioxide (ThO2) is suitable as a model system for more complex materials such as UO2 and its mixed oxides, we present a theoretical investigation of thermal conductivity reduction seen in defect-bearing thorium dioxide and compare directly to experimental measurements. Phonon-mediated thermal transport of the fuel is modeled by a solution to the Boltzmann transport equation (BTE) for phonons. A cluster dynamics (CD) model for lattice defect evolution during irradiation predicts defect densities which are used as input to the BTE for modeling phonon-defect scatterings. Phonon scatterings by lattice defects include those from point defects and vacancy clusters and interstitial clusters of various sizes. The CD model is benchmarked against structural defect characterization of irradiated thorium dioxide using electron microscopy. Thermal conductivity predicted by the BTE model is compared to measured values for irradiated thorium dioxide specimens below room temperature to isolate effects of phonon-defect scattering from intrinsic 3-phonon processes, which dominate at higher temperatures. The computed conductivity values are in partial agreement at temperatures close to room temperature while slight deviations are observed at the lowest measured temperatures, suggesting that implemented phonon-defect scattering cross-section expressions may not be adequate for low temperatures. The presented work provides a necessary investigation of the influence of irradiation induced defects on fuel performance and represents a first step toward a full characterization of phonon mediated thermal transport in irradiated materials with complex defect microstructure.

36 MATERIALS SCIENCE↗