arXiv subjects

Zilong Hua

Publications and source records attributed to Zilong Hua.

10 recordsLinked to original sources

arXiv2026

Thermal Transport in Defective Uranium Nitride: Effects of Point Defects, Anharmonicity, and Electronic Contributions

The impact of point defects on thermal transport in uranium nitride (UN) is investigated using a MLIP combined with Green-Kubo (GK) and normal mode analysis (NMA) methods over 300-1500 K. In pristine UN, temperature-dependent calculations of lattice thermal conductivity reveal that four-phonon scattering is essential yet sufficient to accurately capture high temperature anharmonic phonon transport, as evidenced by close agreement between GK and ShengBTE calculations including three- and four-phonon processes. In defective systems, all types of point defects significantly reduce thermal conductivity at low temperature. Mode-resolved analysis further shows that interstitial defects introduce new phonon states due to a stronger local strain effect. Notably, the uranium interstitial leads to strong defect-phonon scattering over broad phonon spectrum, while the other point defects produce more selective scattering, with even reduced phonon scattering for some acoustic modes. The optical contribution to thermal conductivity remains nearly constant in the presence of IU, but decreases with increasing temperature for pristine and the other defect types. The total thermal conductivity, incorporating electron-phonon coupling and an estimated electronic contribution, yields excellent agreement with experiment in the pristine system, with electronic contributions dominating thermal transport above 600 K. Moreover, with defect-electron contribution introduced through a semiclassical electron-defect scattering model, it is found that (i) the total conductivity degradation follows IU, VU, IN, and VN in descending order, and (ii) electron-phonon coupling becomes negligible in defective systems. These results provide a unified understanding of defect-dependent thermal transport in UN.

cond-mat.mtrl-sci↗

arXiv2025

Machine learning interatomic potential for predicting the thermal properties of uranium nitride

We present a combined computational and experimental investigation of the thermal properties of uranium nitride (UN), focusing on the development of a machine learning interatomic potential (MLIP) using the moment tensor potential (MTP) framework. The MLIP was trained on density functional theory (DFT) data and validated against various quantities including energies, forces, elastic constants, phonon dispersion, and defect formation energies, achieving excellent agreement with DFT calculations, prior experimental results and our thermal conductivity measurement. The potential was then employed in molecular dynamics (MD) simulations to predict key thermal properties such as melting point, thermal expansion, specific heat, and thermal conductivity. To further assess model accuracy, we fabricated a UN sample and performed new thermal conductivity measurements representative of single-crystal properties, which showed strong agreement with the MLIP predictions. This work confirms the reliability and predictive capability of the developed potential for determining the thermal properties of UN.

cond-mat.mtrl-sci↗

arXiv2025

Engineering Phonons in Compositionally Complex Carbide Ceramics

In the pursuit of advanced ceramic materials with exceptional irradiation-resistance and high-temperature tolerance for nuclear applications, compositionally complex carbides (CCCs) have emerged as a highly promising class of candidate materials for extreme environments. In such conditions, critical material properties such as thermal stability, elasticity, thermal conductivity and thermodynamics behavior are predominantly influenced by phonons. In CCCs, pronounced cation disorder can lead to significant phonon scattering due to inherent mass and force constant variations, impacting these critical properties. In this study, we used ab initio calculations to predict the phonon band structures and systematically explore the influence of mass and force constant variance on the phonon spectral function of CCCs with a rock salt structure, ranging from binary to five-metal component carbides. Our findings reveal that the selection and concentration of constituent elements can be strategically utilized to tune the phonon band structure, phonon bandgap and phonon scattering in CCCs, thereby enabling control over phonon-related properties. Additionally, we measured the thermal conductivity of some of these CCCs using the spatial-domain thermoreflectance technique. Interestingly, the measured thermal conductivity of some of these CCCs indicates that five-component ceramics exhibit higher thermal conductivity than certain ternary and binary alloys. This observation contrasts with the expectation that greater cation disorder would result in more scattering and lower thermal conductivity. This intriguing result opens up the possibility of discovering CCCs with better thermal conductivity, presenting new opportunities for their application in extreme environments.

cond-mat.mtrl-sci↗

arXiv2024

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. This study examines the thermal conductivity of a zirconium-doped ThO$_2$ crystal, synthesized via the hydrothermal method using a spatial domain thermo-reflectance 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 Greens 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.

cond-mat.mtrl-sci↗

arXiv2024

Impact of dynamic Jahn-Teller effect on magnetic excitations, lattice vibration, and thermal conductivity in UxTh1-xO2 system

Vibrational and magnetic properties of single-crystal uranium-thorium dioxide (UxTh1-xO2) with a full range of 0<x<1 is investigated. Thorium dioxide is a diamagnet whose thermal properties are governed by lattice vibration. The addition of paramagnetic uranium ion leads to the emergence of magnetic effects that alter the thermophysical properties noticeably even at room temperature. The interaction of phonons with magnetic moments of uranium 5f electrons mediated by magnetoelastic coupling results in an anomalous low-temperature thermal conductivity profile. Analysis of the magnetic susceptibility measurements indicates a uranium-concentration-dependent reduction in effective magnetic moment previously associated with the dynamic Jahn-Teller (DJT) effect. The T2g Raman peak position follows a nonlinear trend as a function of uranium concentration and hints that these Raman active optical modes play a role in either DJT or mediating quadrupole-quadrupole interactions. A first principle-based thermal transport model is implemented to explain the low-temperature transport measurements, where the anomalous reduction is attributed to phonon-spin resonant scattering. The interplay between spins and phonons is also captured using high-resolution inelastic X-ray scattering (IXS) measurements of phonon linewidths. Our results provide new insights into the phonon interactions with the magnetic excitations governing DJT effect and impacting the low-temperature thermal transport processes in this material system. These findings have implications for understanding low-temperature thermal transport and magnetic properties in advanced materials for information processing and energy applications.

cond-mat.str-el↗

arXiv2024

Impacts of Point Defects on Shallow Doping in Cubic Boron Arsenide: A First Principles Study

Cubic boron arsenide (BAs) stands out as a promising material for advanced electronics, thanks to its exceptional thermal conductivity and ambipolar mobility. However, effective control of p- and n-type doping in BAs poses a significant challenge, mostly as a result of the influence of defects. In the present study, we employed density functional theory (DFT) to explore the impacts of the common point defects and impurities on p-type doping of Be$_\text{B}$ and Si$_\text{As}$, and on n-type doping of Si$_\text{B}$ and Se$_\text{As}$. We found that the most favorable point defects formed by C, O, and Si are C$_\text{As}$, O$_\text{B}$O$_\text{As}$, Si$_\text{As}$, C$_\text{As}$Si$_\text{B}$, and O$_\text{B}$Si$_\text{As}$, which have formation energies of less than $1.5$ eV. While the O impurity detrimentally affects both n- and p-type dopings, C and Si impurities are harmful for n-type dopings. Interestingly, the antisite defect pair As$_\text{B}$B$_\text{As}$ benefits both p- and n-type doping. The doping limitation analysis presented in this study can potentially pave the way for strategic development in the area of BAs-based electronics.

cond-mat.mtrl-sci↗

arXiv2023

Thermal conductivity suppression in uranium-doped thorium dioxide due to phonon resonant scattering

In this work, the thermal transport properties of thorium dioxide (ThO$_2$, thoria) with low levels of substitutional uranium (U) doping are explored. We observe strong indications of resonant phonon scattering, an interaction between phonons and electronic degrees of freedom, induced by this doping in addition to common ``impurity'' scattering due to mass and interatomic force constant differences. Uranium doping levels of 6\%, 9\%, and 16\% were studied in a single hydrothermally synthesized U-doped thoria crystal with spatially-varying U doping levels. Within this crystal, isoconcentration regions with relatively uniform doping were located for local thermal conductivity measurements using a thermoreflectance technique. The measured thermal conductivity profiles in the temperature range of 77--300~K are compared to predictions of an analytical Klemens-Callaway thermal conductivity model to identify impacts from different phonon scattering mechanisms. Highly suppressed thermal conductivity at cryogenic temperatures at these doping levels suggests that phonon resonant scattering plays an important role in thermal conductivity reduction in U-doped thoria.

cond-mat.mtrl-sci↗

arXiv2023

Temperature-dependent elastic constants of thorium dioxide probed using time-domain Brillouin scattering

We report the adiabatic elastic constants of single-crystal thorium dioxide over a temperature range of 77 - 350 K. Time-domain Brillouin scattering (TDBS), an all-optical, non-contact picosecond ultrasonic technique, is used to generate and detect coherent acoustic phonons that propagate in the bulk perpendicular to the surface of the crystal. These coherent acoustic lattice vibrations have been monitored in two hydrothermally grown single-crystal thorium dioxide samples along the (100) and (311) crystallographic directions. The three independent elastic constants of the cubic crystal (C11, C12 and C44) are determined from the measured bulk acoustic velocities. The longitudinal wave along the (100) orientation provided a direct measurement of C11. Measurement of C44 and C12 was achieved by enhancing the intensity of quasi-shear mode in a (311) oriented crystal by adjusting the polarization angle relative to the crystal axes. We find the magnitude of softening of the three elastic constants to be ~2.5% over the measured temperature range. Good agreement is found between the measured elastic constants with previously reported values at room temperature, and between the measured temperature-dependent bulk modulus with calculated values. We find that semi-empirical models capturing lattice anharmonicity adequately reproduce the observed trend. We also determine the acoustic Gruneisen anharmonicity parameter from the experimentally derived temperature-dependent bulk modulus and previously reported temperature-dependent values of volume thermal expansion coefficient and heat capacity. This work presents measurements of the temperature-dependent elasticity in single-crystal thorium dioxide at cryogenic temperature and provides a basis for testing ab initio theoretical models and evaluating the impact of anharmonicity on thermophysical properties.

cond-mat.mtrl-sci↗

arXiv2022

Thermal conductivity reduction in (Zr$_{0.25}$Ta$_{0.25}$Nb$_{0.25}$Ti$_{0.25}$)C high entropy carbide from extrinsic lattice defects

High entropy carbides ceramics with randomly-distributed multiple principal cations have shown high temperature stability, low thermal conductivity, and possible radiation tolerance. While chemical disorder has been shown to suppress thermal conductivity in these materials, little investigation has been made on the effects of additional, extrinsically-generated structural defects on thermal transport. Here, (Zr$_{0.25}$Ta$_{0.25}$Nb$_{0.25}$Ti$_{0.25}$)C is exposed to Zr ions to generate a micron-scale, structural-defect-bearing layer. The reduction in lattice thermal transport is measured using laser thermoreflectance. Conductivity changes from different implantation temperatures suggest dislocation loops contribute little to phonon scattering while nanoscale defects serve as effective scatterers, offering a pathway for thermal engineering.

cond-mat.mtrl-sci↗

arXiv2020

Magnetic, transport, and thermal properties of $δ$-phase UZr$_2$

Alloys of hexagonal $δ$-phase UZr$_2$ have been synthesized and studied by means of heat capacity, magnetic susceptibility, magnetization, electrical resistivity, magnetoresistance, thermoelectric power, thermal conductivity measurements, for the first time, at temperatures from 1.8 to 300 K and in magnetic fields up to 8 T. The weak temperature dependence of the magnetic susceptibility and the small value of both Seebeck (0.75 $μ$V/K at room temperature) and of the Sommerfeld coefficient (13.5 mJ mol$^{-1}$ K$^{-2}$) point to 5$f$-electrons in this material having a delocalized nature. The electrical resistivity and magnetoresistance indicate the presence of significant electronic disorder in $δ$-UZr$_2$, consistent with the disorder in its crystal structure. Density functional theory calculations have been performed and compared to experimental results.

cond-mat.str-el↗