Two-temperature pair potentials and phonon spectra for simple metals in the warm dense matter regime

We develop ion-ion pair potentials for Al, Na and K for densities and temperatures relevant to the warm-dense-matter (WDM) regime. Furthermore, we emphasize non-equilibrium states where the ion temperature $T_i$ differs from the electron temperature $T_e$. This work focuses mainly on ultra-fast laser-metal interactions where the energy of the laser is almost exclusively transferred to the electron sub-system over femtosecond time scales. This results in a two-temperature system with $T_e>T_i$ and with the ions still at the initial room temperature $T_i=T_r$. First-principles calculations, such as density functional theory (DFT) or quantum Monte Carlo, are as yet not fully feasible for WDM conditions due to lack of finite-$T$ features, e.g. pseudopotentials, and extensive CPU time requirements. Simpler methods are needed to study these highly complex systems. We propose to use two-temperature pair potentials $U_{ii}(r, T_i,T_e)$ constructed from linear-response theory using the non-linear electron density $n(\mathbf{r})$ obtained from finite-$T$ DFT with a single ion immersed in the appropriate electron fluid. We compute equilibrium phonon spectra at $T_r$ which are found to be in very good agreement with experiments. This gives credibility to our non-equilibrium phonon dispersion relations which are important in determining thermophysical properties, stability, energy-relaxation mechanisms and transport coefficients.Comment: International Conf. on Strongly-Coupled Coulombo Systems (SCCS) 201

Isochoric, isobaric and ultrafast conductivities of aluminum, lithium and carbon in the warm dense matter (WDM) regime

We study the conductivities $\sigma$ of (i) the equilibrium isochoric state ($\sigma_{\rm is}$), (ii) the equilibrium isobaric state ($\sigma_{\rm ib}$), and also the (iii) non-equilibrium ultrafast matter (UFM) state ($\sigma_{\rm uf}$) with the ion temperature $T_i$ less than the the electron temperature $T_e$. Aluminum, lithium and carbon are considered, being increasingly complex warm dense matter (WDM) systems, with carbon having transient covalent bonds. First-principles calculations, i.e., neutral-pseudoatom (NPA) calculations and density-functional theory (DFT) with molecular-dynamics (MD) simulations, are compared where possible with experimental data to characterize $\sigma_{\rm ic}, \sigma_{\rm ib}$ and $\sigma_{\rm uf}$. The NPA $\sigma_{\rm ib}$ are closest to the available experimental data when compared to results from DFT+MD, where simulations of about 64-125 atoms are typically used. The published conductivities for Li are reviewed and the value at a temperature of 4.5 eV is examined using supporting X-ray Thomson scattering calculations. A physical picture of the variations of $\sigma$ with temperature and density applicable to these materials is given. The insensitivity of $\sigma$ to $T_e$ below 10 eV for carbon, compared to Al and Li, is clarified.Comment: 10 figure

Ion-ion dynamic structure factor, acoustic modes and equation of state of two-temperature warm dense aluminum

The ion-ion dynamical structure factor and the equation of state of warm dense aluminum in a two-temperature quasi-equilibrium state, with the electron temperature higher than the ion temperature, are investigated using molecular-dynamics simulations based on ion-ion pair potentials constructed from a neutral pseudoatom model. Such pair potentials based on density functional theory are parameter-free and depend directly on the electron temperature and indirectly on the ion temperature, enabling efficient computation of two-temperature properties. Comparison with ab initio simulations and with other average-atom calculations for equilibrium aluminum shows good agreement, justifying a study of quasi-equilibrium situations. Analyzing the van Hove function, we find that ion-ion correlations vanish in a time significantly smaller than the electron-ion relaxation time so that dynamical properties have a physical meaning for the quasi-equilibrium state. A significant increase in the speed of sound is predicted from the modification of the dispersion relation of the ion acoustic mode as the electron temperature is increased. The two-temperature equation of state including the free energy, internal energy and pressure is also presented

Intranet and internet uptake and usage within UK building surveying practices. A user based evaluation of advantages and disadvantages

The &lsquo;single most important technological discovery since the birth of the p.c.&rsquo;, (Gates, 1996). The swift increase in Internet utilisation within businesses and surveying has changed working methods within UK based Surveying practices. User numbers expanded rapidly since the early 1990&rsquo;s and estimates place a figure of 150 million internet users globally (www.Yahoo.com, 2000). Sloan and Kee Low (2000) established that &lsquo;e-commerce&rsquo; is a revolutionary way of trading and conducting business activities. There are opportunities for surveying practices including, reducing communication time, increasing revenues from new and existing sources, enhanced client satisfaction and competitive advantage (Cronin, 1996). Others (Dixon, 1998) perceive threats, such as &lsquo;disintermediation&rsquo;, to the traditional role of the surveyor.This research examined the levels of internet and intranet access within the UK Building and Quantity Surveying practices and corporate firms to establish how the internet has affected working methods and client requirements. The research method comprised a qualitative approach using an email and postal questionnaire survey of a random sample of practices. The questionnaire findings formed the basis of semi structured interviews conducted with senior management of large practices to gain a deeper understanding of the issues identified within the survey.Data analysis revealed the traditional role of the surveyor as a broker of information may be under threat in the long term. Generally levels of internet access in the sample exceed that of general business levels (Dti, 2000) with the largest growth pre 1997. The perceived advantages and barriers to Intranet and Internet usage were identified by the research.<br /

PRETREATMENT OF TC CONTAINING WASTE AND ITS EFFECT ON 99 TC LEACHING FROM GROUTS

A salt solution (doped with Tc-99), that simulates the salt waste stream to be processed at the Saltstone Production Facility, was immobilized in grout waste forms with and without (1) ground granulated blast furnace slag and (2) pretreatment with iron salts. The degree of immobilization of Tc-99 was measured through monolithic and crushed grout leaching tests. Although Fe (+2) was shown to be effective in reducing Tc-99 to the +4 state, the strong reducing nature of the blast furnace slag present in the grout formulation dominated the reduction of Tc-99 in the cured grouts. An effective diffusion coefficient of 4.75 x 10{sup -12} (Leach Index of 11.4) was measured using the ANSI/ANS-16.1 protocol. The leaching results show that, even in the presence of a concentrated salt solution, blast furnace slag can effectively reduce pertechnetate to the immobile +4 oxidation state. The measured diffusivity was introduced into a flow and transport model (PORFLOW) to calculate the release of Tc-99 from a Saltstone Vault as a function of hydraulic conductivity of the matrix

Characterization of Slag, Fly Ash and Portland Cement for Saltstone

Batch-to-batch variability in the chemical and physical properties of the fly ash, slag and portland cement (binders) will be an ongoing concern over the many years that salt waste from Tank 50 will be processed into grout at the Saltstone Processing Facility. This batch-to-batch variability in the properties of the binder materials translates to variability in the fresh and cured properties of Saltstone. Therefore, it is important to quantify the batch-to-batch variability of the binder materials and the resultant variation in grout properties. This report is the starting point for that process by providing the baseline (reference point) binder properties to which future batches of binder materials can be compared. For this characterization effort, properties of fly ash, slag and portland cement were obtained and documented in this report. These properties included particle size distribution by laser light scattering and dry sieving, particle size and morphology by scanning electron microscopy, true, aerated and tapped densities, chemical composition, rheological properties of the water based slurries made from individual binder material, and volatility through thermogravimetric analysis and differential thermal analysis. The properties presented in this report also provide a baseline data set to assist in problem solving efforts when or if unanticipated and/or unwanted processing events occur at the Saltstone Processing Facility

INTERNATIONAL PROGRAM: SUMMARY REPORT ON THE PROPERTIES OF CEMENTITIOUS WASTE FORMS

This report provides a summary of the results on the properties of cementitious waste forms obtained as part of the International Program. In particular, this report focuses on the results of Task 4 of the Program that was initially entitled ''Improved Retention of Key Contaminants of Concern in Low Temperature Immobilized Waste Forms''. Task 4 was a joint program between Khlopin Radium Institute and the Savannah River National Laboratory. The task evolved during this period into a study of cementitious waste forms with an expanded scope that included heat of hydration and fate and transport modeling. This report provides the results for Task 4 of the International Program as of the end of FY06 at which time funding for Task 4 was discontinued due to the needs of higher priority tasks within the International Program. Consequently, some of the subtasks were only partially completed, but it was considered important to capture the results up to this point in time. Therefore, this report serves as the closeout report for Task 4. The degree of immobilization of Tc-99 within the Saltstone waste form was measured through monolithic and crushed grout leaching tests. An effective diffusion coefficient of 4.8 x 10{sup -12} (Leach Index of 11.4) was measured using the ANSI/ANS-16.1 protocol which is comparable with values obtained for tank closure grouts using a dilute salt solution. The leaching results show that, in the presence of concentrated salt solutions such as those that will be processed at the Saltstone Production Facility, blast furnace slag can effectively reduce pertechnetate to the immobile +4 oxidation state. Leaching tests were also initiated to determine the degree of immobilization of selenium in the Saltstone waste form. Results were obtained for the upper bound of projected selenium concentration ({approx}5 x 10{sup -3} M) in the salt solution that will be treated at Saltstone. The ANSI/ANS 16.1 leaching tests provided a value for the effective diffusivity of {approx}5 x 10{sup -9} cm{sup 2}/sec and a corresponding leaching index of {approx}8.2. Leaching tests at the lower bound of concentration and the leaching tests to determine the impact of redox (selenium exists in two oxidation states, selenite (SeO{sub 3}{sup -2}) and selenate (SeO{sub 4}{sup -2})) on Se-79 release were not completed due to lack of funding. The heat of hydration of a Saltstone mix limits the processing rate at the Saltstone Production Facility. Therefore, reduction in the heat of hydration of a Saltstone formulation that still complies with the remaining property requirements would provide for a greater rate of production. Initial testing for this task was completed. There was good agreement between the isothermal measurements of heat of hydration performed as part of this task with previous measurements of heat of hydration of Saltstone obtained adiabatically over the same 80 hour time period. The slightly higher heat of hydration per gram of cementitious material measured adiabatically can be explained by the higher temperatures achieved during the adiabatic measurements. The isothermal measurements reveal additional details of the heat generation process that were not evident in the adiabatic measurements. An initial heat release in the first minutes was observed isothermally. A second peak at about 5 hours was also observed isothermally that was not detected adiabatically. The major heat releases in the 10 to 30 hour period were observed by both techniques but at slightly different times and ratios of the two major peaks that comprise that region. The degree of reaction was calculated from these measurements based upon the value assigned to maximum hydration. Using the Schmidt method, the degree of reaction after 80 hours was 36% complete by isothermal calorimetry and 46% complete by adiabatic calorimetry. Using the theoretical maximum wherein the fly ash and slag are hydraulically equivalent to the portland cement, the degree of reaction after 80 hours was 20% complete by isothermal calorimetry and 25% complete by adiabatic calorimetry. This time dependence of the heat of hydration is used at SRNL as input into a model that predicts the temperature rise within the Saltstone vaults. The transport of radionuclides and oxygen within the Saltstone waste form and surrounding concrete vault were calculated using the PORFLOW{trademark} code (Performance Assessment calculations at Savannah River Site also use this commercially available code). The Tc-99 effective diffusivity, obtained through leaching tests, was used as input into the code to predict release of Tc-99 from the waste form and from the vault as a function of time (10,000 year compliance period). A sensitivity study was performed to determine the Tc-99 release as a function of changes to the hydraulic conductivity and effective diffusivity of Tc-99. These results are included in this report