ALBERT

Description: We report the identification of heavy Rydberg resonances in the ion-pair spectra of I 2 , Cl 2 , ICl, and IBr. Extensive vibrational progressions are analysed in terms of the energy dependence of the quantum defect δ( E b ) rather than as Dunham expansions. This is shown to define the heavy Rydberg region, providing a more revealing fit to the data with fewer coefficients and leads just as easily to numbering data sets separated by gaps in the observed vibrational progressions. Interaction of heavy Rydberg states with electronic Rydberg states at avoided crossings on the inner wall of the ion-pair potential is shown to produce distinctive changes in the energy dependence of δ( E b ), with weak and strong interactions readily distinguished. Heavy Rydberg behaviour is found to extend well below near-dissociation states, down to vibrational levels ∼18 000-20 000 cm −1 below dissociation. The rapid semi-classical calculation of δ( E b ) for heavy Rydberg states is emphasised and shows their absolute magnitude to be essentially the volume of phase space excluded from the vibrational motion by avoiding core-core penetration of the ions.

Description: The Prototype Material Plasma Exposure eXperiment (Proto-MPEX) at Oak Ridge National Laboratory (ORNL) is a precursor linear plasma device to the Material Plasma Exposure eXperiment (MPEX), which will study plasma material interactions (PMIs) for future fusion reactors. This paper will discuss the initial steps performed towards completing a power balance on Proto-MPEX to quantify where energy is lost from the plasma, including the relevant diagnostic package implemented. Machine operating parameters that will improve Proto-MPEX’s performance may be identified, increasing its PMI research capabilities.

Description: Understanding the impact and complex interaction of thermal carrier scattering centers in functional oxide systems is critical to their progress and application. In this work, we study the interplay among electron and phonon thermal transport, mass-impurity scattering, and phonon-vacancy interactions on the thermal conductivity of cadmium oxide. We use time domain thermoreflectance to measure the thermal conductivity of a set of CdO thin films doped with Dy up to the saturation limit. Using measurements at room temperature and 80 K, our results suggest that the enhancement in thermal conductivity at low Dy concentrations is dominated by an increase in the electron mobility due to a decrease in oxygen vacancy concentration. Furthermore, we find that at intermediate doping concentrations, the subsequent decrease in thermal conductivity can be ascribed to a large reduction in phononic thermal transport due to both point defect and cation-vacancy scattering. With these results, we gain insight into the complex dynamics driving phonon scattering and resulting thermal transport in functional oxides.

Description: We employ Monte Carlo simulation to examine encapsulation in a system comprising Janus oblate spheroids and isotropic spheres. More specifically, the impact of variations in temperature, particle size, inter-particle interaction range, and strength is examined for a system in which the spheroids act as the encapsulating agents and the spheres as the encapsulated guests. In this picture, particle interactions are described by a quasi-square-well patch model. This study highlights the environmental adaptation and selectivity of the encapsulation system to changes in temperature and guest particle size, respectively. Moreover, we identify an important range in parameter space where encapsulation is favored, as summarized by an encapsulation map. Finally, we discuss the generalization of our results to systems having a wide range of particle geometries.

Description: We present a new hybrid multiconfigurational method based on the concept of range-separation that combines the density matrix renormalization group approach with density functional theory. This new method is designed for the simultaneous description of dynamical and static electron-correlation effects in multiconfigurational electronic structure problems.

Description: Hypervelocity particles, such as meteoroids and space debris, routinely impact spacecraft and are energetic enough to vaporize and ionize themselves and as well as a portion of the target material. The resulting plasma rapidly expands into the surrounding vacuum. While plasma measurements from hypervelocity impacts have been made using ground-based technologies such as light gas guns and Van de Graaff dust accelerators, some of the basic plasma properties vary significantly between experiments. There have been both ground-based and in-situ measurements of radio frequency (RF) emission from hypervelocity impacts, but the physical mechanism responsible and the possible connection to the impact-produced plasma are not well understood. Under certain conditions, the impact-produced plasma can have deleterious effects on spacecraft electronics by providing a new current path, triggering an electrostatic discharge, causing electromagnetic interference, or generating an electromagnetic pulse. Multi-physics simulations of plasma production from hypervelocity impacts are presented. These simulations incorporate elasticity and plasticity of the solid target, phase change and plasma formation, and non-ideal plasma physics due to the high density and low temperature of the plasma. A smoothed particle hydrodynamics method is used to perform a continuum dynamics simulation with these additional physics. By examining a series of hypervelocity impacts, basic properties of the impact produced plasma plume (density, temperature, expansion speed, charge state) are determined for impactor speeds between 10 and 72 km/s. For a large range of higher impact speeds (30–72 km/s), we find the temperature is unvarying at 2.5 eV. We also find that the plasma plume is weakly ionized for impact speeds less than 14 km/s and fully ionized for impact speeds greater than 20 km/s, independent of impactor mass. This is the same velocity threshold for the detection of RF emission in recent Van de Graaff experiments, suggesting that the RF is correlated to the formation of fully ionized plasma.

Description: We study the electron and phonon thermal coupling mechanisms at interfaces between gold films with and without Ti adhesion layers on various substrates via pump-probe time-domain thermoreflectance. The coupling between the electronic and the vibrational states is increased by more than a factor of five with the inclusion of an ∼3 nm Ti adhesion layer between the Au film and the non-metal substrate. Furthermore, we show an increase in the rate of relaxation of the electron system with increasing electron and lattice temperatures induced by the laser power and attribute this to enhanced electron-electron scattering, a transport channel that becomes more pronounced with increased electron temperatures. The inclusion of the Ti layer also results in a linear dependence of the electron-phonon relaxation rate with temperature, which we attribute to the coupling of electrons at and near the Ti/substrate interface. This enhanced electron-phonon coupling due to electron-interface scattering is shown to have negligible influence on the Kapitza conductances between the Au/Ti and the substrates at longer time scales when the electrons and phonons in the metal have equilibrated. These results suggest that only during highly nonequilibrium conditions between the electrons and phonons ( T e ≫ T p ) does electron-phonon scattering at an interface contribute to thermal boundary conductance.

Description: We present here the coupling of a polarizable embedding (PE) model to the recently developed multiconfiguration short-range density functional theory method (MC-srDFT), which can treat multiconfigurational systems with a simultaneous account for dynamical and static correlation effects. PE-MC-srDFT is designed to combine efficient treatment of complicated electronic structures with inclusion of effects from the surrounding environment. The environmental effects encompass classical electrostatic interactions as well as polarization of both the quantum region and the environment. Using response theory, molecular properties such as excitation energies and oscillator strengths can be obtained. The PE-MC-srDFT method and the additional terms required for linear response have been implemented in a development version of Dalton . To benchmark the PE-MC-srDFT approach against the literature data, we have investigated the low-lying electronic excitations of acetone and uracil, both immersed in water solution. The PE-MC-srDFT results are consistent and accurate, both in terms of the calculated solvent shift and, unlike regular PE-MCSCF, also with respect to the individual absolute excitation energies. To demonstrate the capabilities of PE-MC-srDFT, we also investigated the retinylidene Schiff base chromophore embedded in the channelrhodopsin protein. While using a much more compact reference wave function in terms of active space, our PE-MC-srDFT approach yields excitation energies comparable in quality to CASSCF/CASPT2 benchmarks.

Description: In this work, we examine how deuterium becomes trapped in plasma-exposed tungsten and forms near-surface platelet-shaped precipitates. How these bubbles nucleate and grow, as well as the amount of deuterium trapped within, is crucial for interpreting the experimental database. Here, we use a combined experimental/theoretical approach to provide further insight into the underlying physics. With the Tritium Plasma Experiment, we exposed a series of ITER-grade tungsten samples to high flux D plasmas (up to 1.5 × 10 22  m −2  s −1 ) at temperatures ranging between 103 and 554 °C. Retention of deuterium trapped in the bulk, assessed through thermal desorption spectrometry, reached a maximum at 230 °C and diminished rapidly thereafter for T  〉 300 °C. Post-mortem examination of the surfaces revealed non-uniform growth of bubbles ranging in diameter between 1 and 10  μ m over the surface with a clear correlation with grain boundaries. Electron back-scattering diffraction maps over a large area of the surface confirmed this dependence; grains containing bubbles were aligned with a preferred slip vector along the ⟨111⟩ directions. Focused ion beam profiles suggest that these bubbles nucleated as platelets at depths of 200 nm–1  μ m beneath the surface and grew as a result of expansion of sub-surface cracks. To estimate the amount of deuterium trapped in these defects relative to other sites within the material, we applied a continuum-scale treatment of hydrogen isotope precipitation. In addition, we propose a straightforward model of near-surface platelet expansion that reproduces bubble sizes consistent with our measurements. For the tungsten microstructure considered here, we find that bubbles would only weakly affect migration of D into the material, perhaps explaining why deep trapping was observed in prior studies with plasma-exposed neutron-irradiated specimens. We foresee no insurmountable issues that would prevent the theoretical framework developed here from being extended to a broader range of systems where precipitation of insoluble gases in ion beam or plasma-exposed metals is of interest.

Description: Gallium nitride (GaN) is a widely used semiconductor for high frequency and high power devices due to of its unique electrical properties: a wide band gap, high breakdown field, and high electron mobility. However, thermal management has become a limiting factor regarding efficiency, lifetime, and advancement of GaN devices and GaN-based applications. In this work, we study the thermal conductivity of beta-phase gallium oxide ( β -Ga 2 O 3 ) thin films, a component of typical gate oxides used in such devices. We use time domain thermoreflectance to measure the thermal conductivity of a variety of polycrystalline β -Ga 2 O 3 films of different thicknesses grown via open atmosphere annealing of the surfaces of GaN films on sapphire substrates. We show that the measured effective thermal conductivity of these β -Ga 2 O 3 films can span 1.5 orders of magnitude, increasing with an increased film thickness, which is indicative of the relatively large intrinsic thermal conductivity of the β -Ga 2 O 3 grown via this technique (8.8 ± 3.4 W m −1 K −1 ) and large mean free paths compared to typical gate dielectrics commonly used in GaN device contacts. By conducting time domain thermoreflectance (TDTR) measurements with different metal transducers (Al, Au, and Au with a Ti wetting layer), we attribute this variation in effective thermal conductivity to a combination of size effects in the β -Ga 2 O 3 film resulting from phonon scattering at the β -Ga 2 O 3 /GaN interface and thermal transport across the β -Ga 2 O 3 /GaN interface. The measured thermal properties of open atmosphere-grown β -Ga 2 O 3 and its interface with GaN set the stage for thermal engineering of gate contacts in high frequency GaN-based devices.