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DOE OSTI2023

Influence of liquid conductance on the temporal evolution of self-organization patterns in atmospheric pressure DC glow discharges

Abstract Self-Organized Patterns (SOPs) at plasma-liquid interface in atmospheric pressure plasma discharges refer to the formation of intricate and puzzling structures due to the interplay of electrodynamic and hydrodynamic processes. Studies conducted to date have shown that this phenomenon results in the formation of distinctive patterns such as circular ring, star, gear, dots, spikes, etc., and primarily depends on working gas, electrolyte type, gap distance, current, conductivity, etc. However, an adequate understanding of how these patterns change from one type to another is still not available. This study aims to elucidate the influence of initial liquid conductance ( σ i ) on the temporal evolution of SOPs in liquid-anode discharges. The discharge was generated in a pin-to-liquid anode configuration at a constant helium (He) flow rate of 500 sccm and DC applied voltage of 6 kV at a gap distance of 12 mm. Through the gradual increment of σ i from 1.8 μ S to 4820 μ S, we observe that the trend in the evolution of SOPS takes place as solid discs, spikes, dots, rings, double rings, and stars. The continuous formation of reactive species onto the liquid anode in all conductive solutions results in a decrease in pH, an increase in bulk liquid temperature, and an increase in total dissolved solutes, and these have been confirmed through experimental measurements. Observations using optical emission spectroscopy show that the electrons at the plasma-liquid interface participate in the reduction of cations followed by their excitation & ionization due to which electron density as well as emissions from excited species (mainly hydroxyl radicals & excited nitrogen) decrease with time. Our investigation provides experimental evidence on the presence of cations at the plasma-liquid interface required for SOP formation.

Physics↗

DOE OSTI2026

Development of thermal joints for conduction-cooling applications

Abstract In support of the development of conduction-cooled superconducting radiofrequency (SRF) niobium cavities for use in continuous-wave linear accelerators, an experimental study of thermal contact resistance was performed on bolted joints using high-purity niobium, aluminium, and copper along with Apiezon N grease and indium foil as interfacial materials. The geometry of each joint investigated aims at replicating the design adopted in conduction-cooled SRF cavities currently under development at Jefferson Lab. The materials’ thermal conductivity and the joints’ thermal resistance were measured in the temperature range of 3.5 - 10 K. The results showed that the low thermal contact resistance of 2-4 K·cm 2 /W at 4.3 K achieved with Al-In-Nb and Al-Apiezon N-Cu joints should allow the operation of conduction-cooled SRF cavities at a targeted accelerating gradient of ∼10 MV/m.

Lewis, J. [Old Dominion University]↗

DOE OSTI2021

Limitation of C4 photosynthesis by low carbonic anhydrase activity increases with temperature but does not influence mesophyll CO2 conductance

The CO2-concentrating mechanism (CCM) in C4 plants is initiated by the uptake of bicarbonate (HCO3…) via phosphoenolpyruvate carboxylase (PEPC). Generation of HCO3– for PEPC is determined by the interaction between mesophyll CO2 conductance and the hydration of CO2 to HCO3– by carbonic anhydrase (CA). Genetic reduction of CA was previously shown not to limit C4 photosynthesis under ambient atmospheric partial pressures of CO2 (pCO2). However, CA activity varies widely across C4 species and it is unknown if there are specific environmental conditions (e.g. high temperature) where CA may limit HCO3– production for C4 photosynthesis. Additionally, CA activity has been suggested to influence mesophyll conductance, but this has not been experimentally tested. We hypothesize that CA activity can limit PEPC at high temperatures, particularly at low pCO2, but does not directly influence gm. Here we tested the influence of genetically reduced CA activity on photosynthesis and gm in the C4 plant Zea mays under a range of pCO2 and temperatures. Reduced CA activity limited HCO3– production for C4 photosynthesis at low pCO2 as temperatures increased, but did not influence mesophyll conductance. Therefore, high leaf CA activity may enhance C4 photosynthesis under high temperature when stomatal conductance restricts the availability of atmospheric CO2.

Plant Sciences↗

DOE OSTI2026

Four-Dimensional Quasielastic Neutron Scattering (4D-QENS) Analysis of Correlated Ionic Conduction in Sr⁢Cl2

Methods of elucidating the mechanisms of fast-ion conduction in solid-state materials are pivotal for advancements in energy technologies such as batteries, fuel cells, sensors, and supercapacitors. In this study, we examine the ionic conduction pathways in single crystal Sr⁢Cl2, which is a fast-ion conductor above 900 K, using four-dimensional quasielastic neutron scattering (4D-QENS). We explore both coherent and incoherent neutron scattering at temperatures above the transition temperature into the superionic phase to explore the correlated motion of hopping anions. Refinements of the incoherent QENS yield residence times and jump probabilities between lattice sites in good agreement with previous studies, confirming that ionic hopping along nearest-neighbor directions is the most probable conduction pathway. However, the coherent QENS reveals evidence of de Gennes narrowing, indicating the importance of ionic correlations in the conduction mechanism. This highlights the need for improvements both in the theory of ionic transport in fluorite compounds and the modeling of coherent 4D-QENS in single crystals.

Coles, Jared [Materials Science Division, Argonne ↗

DOE OSTI2023

Impacts of irradiation-induced nanostructure on phonon linewidths and thermal conductivity in U-Zr alloy

Ion irradiation can significantly change material properties. Thermal conductivity degradation of reactor fuel is detrimental to safety and efficiency—driving research on how irradiation impacts heat-carrying phonons. Here, we report the measurements of phonon dispersion and lifetimes (inverse linewidths) in freestanding irradiated crystals and reveal the relationship between thermal conductivity and proton irradiation induced nanostructures in UZr 2.6 using inelastic x-ray scattering, electron microscopy, modulated thermoreflectance, and first-principles calculations. Irradiation results in more significant increases in phonon linewidths and decreased thermal conductivity in the basal plane than that along the c axis, decreasing thermal conductivity anisotropy. Furthermore, microscopy reveals that this results from irradiation induced nanoprecipitates and metastable phase separation. Surprisingly, irradiation leads to smaller phonon linewidths near some zone boundaries, which we attribute to irradiation induced short-range order.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Optical conductivity of overdoped cuprates from ab initio out-of-plane impurity potentials

Dopant impurity potentials determined by ab initio supercell density functional theory calculations are used to calculate the optical conductivity of overdoped La 2-x ⁢Sr x CuO 4 (LSCO) and Tl 2 ⁢Ba 2⁢ CuO 6+δ (Tl-2201) in the superconducting and normal states. Vertex corrections are included to account for the effect of forward scattering on two-particle properties. This approach was previously shown to provide good, semiquantitative agreement with measurements of superfluid density in LSCO. Here, in this study, we compare calculations of conductivity with measurements of terahertz conductivity on LSCO using identical impurity, band, and correlation parameters and find similarly good correspondence with experiment. In the process, we delineate the impact of the different disorder mechanisms on single-particle and transport relaxation processes. In particular, we reveal the critical role of apical oxygen vacancies in transport scattering and show that transport relaxation rates in LSCO are significantly reduced when apical oxygen vacancies are annealed out. These considerations are shown to be crucial for understanding the variability of experimental results for overdoped LSCO in samples of nominally identical doping but different types. Finally, we give predictions for Tl-2201 terahertz conductivity experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2013

Minimum thermal conductivity in superlattices: A first-principles formalism

The thermal conductivity of silicon-germanium superlattices is computed here from density-functional perturbation theory using relaxation times that include both anharmonic and interface roughness effects. A decrease in the group velocity of low-frequency phonons in addition to the interface-disorder-induced scattering of high-frequency phonons drives the superlattice thermal conductivity to below the alloy limit. At short periods, interplay between decrease in group velocity and increase in phonon lifetimes with increase in superlattice period leads to a minimum in the cross-plane thermal conductivity. Increasing the mass mismatch between the constituent materials in the superlattice further lowers the thermal conductivity below the alloy limit, pointing to avenues for higher efficiency thermoelectric materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

Temperature-dependent thermal conductivity in silicon nanostructured materials studied by the Boltzmann transport equation

Nanostructured materials show low thermal conductivity because of the additional scattering due to phonon-boundary interactions. As these interactions are highly sensitive to the mean free path (MFP) of phonons, MFP distributions in nanostructures can be dramatically distorted relative to bulk. Here we calculate the MFP distribution in periodic nanoporous Si for different temperatures, using the recently developed MFP-dependent Boltzmann transport equation. After analyzing the relative contribution of each phonon branch to thermal transport in nanoporous Si, we find that at room temperature optical phonons contribute 17 % to heat transport, compared to 5 % in bulk Si. Interestingly, we observe a constant thermal conductivity over the range 200 K < T < 300 K . Furthermore, we attribute this behavior to the ballistic transport of acoustic phonons with long intrinsic MFP and the temperature dependence of the heat capacity. Our findings, which are in qualitative agreement with the temperature trend of thermal conductivities measured in nanoporous Si-based systems, shed light on the origin of the reduction of thermal conductivity in nanostructured materials and demonstrate the necessity of multiscale heat transport engineering, in which the bulk material and geometry are optimized concurrently.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Estimates of crystalline LiF thermal conductivity at high temperature and pressure by a Green-Kubo method

Here, given the unique optical properties of LiF, it is often used as an observation window in high-temperature and -pressure experiments; hence, estimates of its transmission properties are necessary to interpret observations. Since direct measurements of the thermal conductivity of LiF at the appropriate conditions are difficult, we resort to molecular simulation methods. Using an empirical potential validated against ab initio phonon density of states, we estimate the thermal conductivity of LiF at high temperatures (1000–4000 K) and pressures (100–400 GPa) with the Green-Kubo method. We also compare these estimates to those derived directly from ab initio data. To ascertain the correct phase of LiF at these extreme conditions, we calculate the (relative) phase stability of the B1 and B2 structures using a quasiharmonic ab initio model of the free energy. We also estimate the thermal conductivity of LiF in an uniaxial loading state that emulates initial stages of compression in high-stress ramp loading experiments and show the degree of anisotropy induced in the conductivity due to deformation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

Chemical pressure effect on the optical conductivity of the nodal-line semimetals ZrSi Y ( Y = S,Se,Te) and ZrGe Y ( Y = S,Te)

ZrSiS is a nodal-line semimetal, whose electronic band structure contains a diamond-shaped line of Dirac nodes. We carried out a comparative study on the optical conductivity of ZrSiS and the related compounds ZrSiSe, ZrSiTe, ZrGeS, and ZrGeTe by reflectivity measurements over a broad frequency range combined with density functional theory calculations. The optical conductivity exhibits a distinct U shape, ending at a sharp peak at around 10 000 cm –1 for all studied compounds except for ZrSiTe. The U shape of the optical conductivity is due to transitions between the linearly dispersing bands crossing each other along the nodal line. The sharp high-energy peak is related to transitions between almost parallel bands, and its energy position depends on the interlayer bonding correlated with the c/a ratio, which can be tuned by either chemical or external pressure. For ZrSiTe, another pair of crossing bands appears in the vicinity of the Fermi level, corrugating the nodal-line electronic structure and leading to the observed difference in optical conductivity. Here, the findings suggest that the Dirac physics in ZrXY compounds with X = Si,Ge and Y = S,Se,Te is closely connected to the interlayer bonding.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Electrical conductivity of a warm neutron star crust in magnetic fields: Neutron-drip regime

We compute the anisotropic electrical conductivity tensor of the inner crust of a compact star at nonzero temperature by extending a previous work on the conductivity of the outer crust. The physical scenarios, where such crust is formed, involve protoneutron stars born in supernova explosions, binary neutron star mergers, and accreting neutron stars. The temperature-density range studied covers the transition from a semidegenerate to a highly degenerate electron gas and assumes that the nuclei form a liquid, i.e., the temperature is above the melting temperature of the lattice of nuclei. The electronic transition probabilities include (i) the screening of electron-ion interaction in the hard-thermal-loop approximation for the QED plasma, (ii) the correlations of the ionic component in a one-component plasma, and (iii) finite nuclear size effects. The conductivity tensor is obtained from the Boltzmann kinetic equation in relaxation time approximation accounting for the anisotropy introduced by a magnetic field. The sensitivity of the results towards the matter composition of the inner crust is explored by using several compositions of the inner crust, which were obtained using different nuclear interactions and methods of solving the many-body problem. The standard deviations of relaxation time and components of the conductivity tensor from the average are below ≤25% except close to crust-core transition, where nonspherical nuclear structures are expected. Finally, our results can be used in dissipative magnetohydrodynamics simulations of warm compact stars.

Physics↗

DOE OSTI2020

Correlations between conduction electrons in dense plasmas

Most treatments of electron-electron correlations in dense plasmas either ignore them entirely (random phase approximation) or neglect the role of ions (jellium approximation). In this work, we go beyond both these approximations to derive a formula for the electron-electron static structure factor which properly accounts for the contributions of both ionic structure and quantum-mechanical dynamic response in the electrons. The result can be viewed as a natural extension of the quantum Ornstein-Zernike theory of ionic and electronic correlations, and it is suitable for dense plasmas in which the ions are classical and the conduction electrons are quantum-mechanical. Here, the corresponding electron-electron pair distribution functions are compared with the results of path integral Monte Carlo simulations, showing good agreement whenever no strong electron resonance states are present. We construct approximate potentials of mean force which describe the effective screened interaction between electrons. Significant deviations from Debye-Hückel screening are present at temperatures and densities relevant to high-energy density experiments involving warm and hot dense plasmas. The presence of correlations between conduction electrons is likely to influence the electron-electron contribution to the electrical and thermal conductivity. It is expected that excitation processes involving the conduction electrons (e.g., free-free absorption) will also be affected.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Thermal conductivity of a laser plasma

Here, we present a model of the electron thermal conductivity of a laser-produced plasma. The model, supported by Vlasov–Fokker–Planck simulations, predicts that laser absorption reduces conductivity by forcing electrons out of a Maxwell–Boltzmann equilibrium, which results in depletion of both low-velocity bulk electrons and high-velocity tail electrons. We show that both the bulk and tail electrons approximately follow super-Gaussian distributions, but with distinct exponents that each depend on the laser intensity and wavelength through the parameter a = Zv$^{2}_{E}$/v$^{2}_{T}$. For a value of a = 0.5, tail depletion reduces the thermal conductivity to half its zero-intensity value. We present our results as simple analytic fits that can be readily implemented in any radiation-hydrodynamics code or used to correct the local limit of non-local conduction models.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2015

Anomalous transport on regular fracture networks: Impact of conductivity heterogeneity and mixing at fracture intersections

We investigate here transport on regular fracture networks that are characterized by heterogeneity in hydraulic conductivity. We discuss the impact of conductivity heterogeneity and mixing within fracture intersections on particle spreading. We show the emergence of non-Fickian transport due to the interplay between the network conductivity heterogeneity and the degree of mixing at nodes. Specifically, lack of mixing at fracture intersections leads to subdiffusive scaling of transverse spreading but has negligible impact on longitudinal spreading. An increase in network conductivity heterogeneity enhances both longitudinal and transverse spreading and leads to non-Fickian transport in longitudinal direction. Based on the observed Lagrangian velocity statistics, we develop an effective stochastic model that incorporates the interplay between Lagrangian velocity correlation and velocity distribution. The model is parameterized with a few physical parameters and is able to capture the full particle transition dynamics.

58 GEOSCIENCES↗

DOE OSTI2018

Effects of axial boundary conductivity on a free Stewartson-Shercliff layer

The effects of axial boundary conductivity on the formation and stability of a magnetized free Stewartson-Shercliff layer (SSL) in a short Taylor-Couette device are reported. As the axial field increases with insulating endcaps, hydrodynamic Kelvin-Helmholtz-type instabilities set in at the SSLs of the conducting fluid, resulting in a much reduced flow shear. With conducting endcaps, SSLs respond to an axial field weaker by the square root of the conductivity ratio of endcaps to fluid. Flow shear continuously builds up as the axial field increases despite the local violation of the Rayleigh criterion, leading to a large number of hydrodynamically unstable modes. In conclusion, numerical simulations of both the mean flow and the instabilities are in agreement with the experimental results.

42 ENGINEERING↗

DOE OSTI2016

Proton Conductivity in Phosphoric Acid: The Role of Quantum Effects

Phosphoric acid has one of the highest intrinsic proton conductivities of any known liquids, and the mechanism of this exceptional conductivity remains a puzzle. In our detailed experimental studies we discovered a strong isotope effect in the conductivity of phosphoric acids caused by (i) a strong isotope shift of the glass transition temperature and (ii) a significant reduction of the energy barrier by zero-point quantum fluctuations. Our results suggest that the high conductivity in phosphoric acids is caused by a very efficient proton transfer mechanism, which is strongly assisted by quantum effects.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2017

Resonances in the Field-Angle-Resolved Thermal Conductivity of CeCoIn 5

Here, the thermal conductivity measurement in a rotating magnetic field is a powerful probe of the structure of the superconducting energy gap. We present high-precision measurements of the low-temperature thermal conductivity in the unconventional heavy-fermion superconductor CeCoIn 5 , with the heat current J along the nodal [110] direction of its d x 2 –y 2 order parameter and the magnetic field up to 7 T rotating in the ab plane. In contrast to the smooth oscillations found previously for J∥[100], we observe a sharp resonancelike peak in the thermal conductivity when the magnetic field is also in the [110] direction, parallel to the heat current. We explain this peak qualitatively via a model of the heat transport in a d-wave superconductor. In addition, we observe two smaller but also very sharp peaks in the thermal conductivity for the field directions at angles Θ≈±33° with respect to J. The origin of the observed resonances at Θ≈±33° at present defies theoretical explanation. The challenge of uncovering their source will dictate exploring theoretically more complex models, which might include, e.g., fine details of the Fermi surface, Andreev bound vortex core states, a secondary superconducting order parameter, and the existence of gaps in spin and charge excitations.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Quantization of the Thermal Hall Conductivity at Small Hall Angles

We consider the effect of coupling between phonons and a chiral Majorana edge in a gapped chiral spin liquid with Ising anyons (e.g., Kitaev’s non-Abelian spin liquid on the honeycomb lattice). This is especially important in the regime in which the longitudinal bulk heat conductivity κ x x due to phonons is much larger than the expected quantized thermal Hall conductance $κ$ $^{q}_{xy}$ = (πT/12)($k$ $^{2}_{B}$/ℏ) of the ideal isolated edge mode, so that the thermal Hall angle, i.e., the angle between the thermal current and the temperature gradient, is small. By modeling the interaction between a Majorana edge and bulk phonons, we show that the exchange of energy between the two subsystems leads to a transverse component of the bulk current and thereby an effective Hall conductivity. Remarkably, the latter is equal to the quantized value when the edge and bulk can thermalize, which occurs for a Hall bar of length L >> ℓ, where ℓ is a thermalization length. We obtain ℓ ~ T –5 for a model of the Majorana-phonon coupling. We also find that the quality of the quantization depends on the means of measuring the temperature and, surprisingly, a more robust quantization is obtained when the lattice, not the spin, temperature is measured. We present general hydrodynamic equations for the system, detailed results for the temperature and current profiles, and an estimate for the coupling strength and its temperature dependence based on a microscopic model Hamiltonian. Furthermore, our results may explain recent experiments observing a quantized thermal Hall conductivity in the regime of small Hall angle, κ xy /κ xx ~ 10 –3 , in α–RuCl 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗