An efficient implementation of the direct-SCF algorithm on parallel computer architectures

Summary The development and implementation of a parallel direct self consistent field (SCF) Hartree-Fock algorithm, with gradients and random phase approximation solutions is presented. Important details of the structure of the parallel version of DISCO and preliminary results for calculations using the Concurrent Supercomputing Consortium Intel Touchstone Delta parallel computer system are reported. The data show that the algorithms are efficiently parallelized and that throughput of a one processor CRAY X-MP is reached with about 16 nodes on the Delta. The data also indicate sequential code which was not a bottleneck on traditional supercomputers, can become time critical on parallel computers.This work was performed under the auspices of the Office of Basic Energy Sciences, Division of Chemical Sciences, U.S. Department of Energy, under contract DE-AC06-76RLO 1830 for Pacific Northwest Laboratory which is operated by Battelle Memorial Institute for the U.S. Department of Energy.     

Performance visualization for parallel programs

Summary We describe here a set of graphical performance visualization tools that have been developed at Argonne National Laboratory for increasing one's understanding of the behavior of parallel programsThis work was supported by the Applied Mathematical Sciences subprogram of the Office of Energy Research, U.S. Department of Energy, under contract W-31-109-Eng-38     

On the role of parallel architecture supercomputers in time-dependent approaches to quantum scattering

Summary Results of our initial study of the use of parallel architecture super-computers in solving time-dependent quantum scattering equations are reported. The specific equations solved are obtained from the time-dependent Lippmann-Schwinger integral equation by means of a quadrature approximation to the time integral. This leads to a modified Cayley transform algorithm in which the primary computational step is a matrix-vector multiplication. Implementation has been carried out both for the MasPar MP-1 and the NCUBE 6400 parallel machines. The codes are written in a modular form that greatly facilitates porting from one machine architecture to another. Both parallel machines prove to be more powerful for this application than the serial architecture VAX 8650. Specific analysis of machine performance is given.Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. 2-7405-ENG-82. This research was supported by the Division of Chemical Sciences and Applied Mathematical Sciences, Office of Basic Energy SciencesR.A. Welch Predoctoral Fellow under R.A. Welch Foundation Grant E-608Supported in part under National Science Foundation Grant CHE89-07429     

Parallel direct four-index transformations

Summary Two parallel direct integral transformation algorithms are presented. Specific attention is directed to producing transformed integrals containing at least two active orbital indices. The number of active orbitals is typically much less than the total number of molecular orbitals reflecting the requirements of a wide range of correlated electronic structure methods. Sample direct second-order Møller-Plesset theory calculations are reported. For situations where multipassing of the integrals is required, superlinear speedup is obtained by exploiting the increase in global memory. As a consequence, for morphine in a 6-31G basis, a speedup of over 25 is observed in scaling from 32 to 512 processors.Pacific Northwest Laboratory is operated for the U.S. Department of Energy by Battelle Memorial Institute under contract DE-AC06-76RL0 1830     

Modulated differential scanning calorimetry in the glass transition region

Temperature-modulated calorimetry (TMC) allows the experimental evaluation of the kinetic parameters of the glass transition from quasi-isothermal experiments. In this paper, model calculations based on experimental data are presented for the total and reversing apparent heat capacities on heating and cooling through the glass transition region as a function of heating rate and modulation frequency for the modulated differential scanning calorimeter (MDSC). Amorphous poly(ethylene terephthalate) (PET) is used as the example polymer and a simple first-order kinetics is fitted to the data. The total heat flow carries the hysteresis information (enthalpy relaxation, thermal history) and indications of changes in modulation frequency due to the glass transition. The reversing heat flow permits the assessment of the first and higher harmonics of the apparent heat capacities. The computations are carried out by numerical integrations with up to 5000 steps. Comparisons of the calculations with experiments are possible. As one moves further from equilibrium, i.e. the liquid state, cooperative kinetics must be used to match model and experiment.On leave from Toray Industries, Inc., Otsu, Shiga 520, Japan.This work was supported by the Division of Materials Research, National Science Foundation, Polymers Program, Grant # DMR 90-00520 and the Division of Materials Sciences, Office of Basic Energy Sciences, U. S. Department of Energy at Oak Ridge National Laboratory, managed by Lockheed Martin Energy Research Corp. for the U. S. Department of Energy, under contract number DE-AC05-96OR22464. Support for instrumentation came from TA Instruments, Inc. Research support was also given by ICI Paints, and Toray Industries, Inc.     

Cell asymmetry correction for temperature modulated differential scanning calorimetry

The quality of measurement of heat capacity by differential scanning calorimetry (DSC) is based on strict symmetry of the twin calorimeter. This symmetry is of particular importance for temperature-modulated DSC (TMDSC) since positive and negative deviations from symmetry cannot be distinguished in the most popular analysis methods. The heat capacities for sapphire-filled and empty aluminum calorimeters (pans) under designed cell imbalance caused by different pan-masses were measured. In addition, the positive and negative signs of asymmetry have been explored by analyzing the phase-shift between temperature and heat flow for sapphire and empty runs. The phase shifts change by more than 180° depending on the sign of the asymmetry. Once the sign of asymmetry is determined, the asymmetry correction for temperature-modulated DSC can be made.On leave from Toray Research Center, Inc., Otsu, Shiga 520, JapanThis work was supported by the Division of Materials Research, National Science Foundation, Polymers Program, Grant # DMR 90-00520 and the Division of Materials Sciences, Office of Basic Energy Sciences, U.S. Department of Energy at Oak Ridge National Laboratory, managed by Lockheed Martin Energy Research Corp. for the U.S. Department of Energy, under contract number DE-AC05-960R22464.     

Enthalpies and temperatures of transformation for plutonium using a differential scanning calorimeter

The enthalpies and temperatures of transformation of high purity plutonium were measured using a differential scanning calorimeter. The results of our study are presented and compared to values obtained by previous methods.Work performed under the auspices of the U. S. Department of Energy by Lawrence Livermore Laboratory under contract No. W-7405-Eng-48.     

Determination of cell asymmetry in temperature-modulated DSC

The quality of measurement of heat capacity by differential scanning calorimetry (DSC) is based on the symmetry of the twin calorimeters. This symmetry is of particular importance for the temperature-modulated DSC (TMDSC) since positive and negative deviations from symmetry cannot be distinguished in the most popular analysis methods. Three different DSC instruments capable of modulation have been calibrated for asymmetry using standard non-modulated measurements and a simple method is described that avoids potentially large errors when using the reversing heat capacity as the measured quantity. It consists of overcompensating the temperature-dependent asymmetry by increasing the mass of the sample pan.On leave from Toray Industries, Inc., Otsu, Shiga 520, JapanOn leave from Toray Research Center, Inc., Otsu, Shiga 520, JapanThis work was supported by the Division of Materials Research, National Science Foundation, Polymers Program, Grant # DMR 90-00520 and the Division of Materials Sciences, Office of Basic Energy Sciences, U. S. Department of Energy at Oak Ridge National Laboratory, managed by Lockheed Martin Energy Research Corp. for the U. S. Department of Energy, under contract number DE-AC0S-96OR22464. Support for instrumentation came from TA Instruments, Inc. and Mettler-Toledo, Research support was also given by ICI Painls, and Toray Industries, Inc.     

Fabrication of 50-mg252Cf neutron sources for the FDA activation analysis facility

The Transuranium Processing Plant (TPP) at the Oak Ridge National Laboratory (ORNL) has been requested by the Food and Drug Administration (FDA) to furnish 200 mg of²⁵²Cf for use in their new activation analysis facility. This paper discusses the procedure to be employed in fabricating the californium into four neutron sources, each containing a nominal 50-mg of²⁵²Cf. The completed neutron sources will be assayed using a precision fast-neutron counter, decontaminated and loaded into a concreete-shielded shipping container weighing 10.7 Mg for shipment to the FDA facility located at Howard University in Washington, D. C.Research sponsored by the Office of Basic Energy Sciences, U. S. Department of Energy, under contract DE-AC05-840R21400 with Martin Marietta Energy Systems, Inc.     

Stabilization of divalent californium in crystalline strontium tetraborate

The divalent oxidation state of californium (Cf) has been stabilized in crystalline SrB₄O₇. The ability to generate this less-stable oxidation state in an oxide matrix is significant. Factors promoting this stabilization have been determined. Access to this divalent state and those of many other lanthanide and actinide elements via a rather straightforward laboratory procedure now facilitates their study and characterization.Research sponsored by the Division of Chemical Sciences, Office of Basic Energy Sciences, U.S. Department of Energy under grant DE-FG05-88ER13865 to the University of Tennessee, Knoxville and contract DE-AC05-84OR21400 with Martin Marietta Energy Systems, Inc.     

Investigating the performance of parallel eigensolvers for large processor counts

Summary Eigensolving (diagonalizing) small dense matrices threatens to become a bottleneck in the application of massively parallel computers to electronic structure methods. Because the computational cost of electronic structure methods typically scales asO(N ³) or worse, even teraflop computer systems with thousands of processors will often confront problems withN 10,000. At present, diagonalizing anN×N matrix onP processors is not efficient whenP is large compared toN. The loss of efficiency can make diagonalization a bottleneck on a massively parallel computer, even though it is typically a minor operation on conventional serial machines. This situation motivates a search for both improved methods and identification of the computer characteristics that would be most productive to improve.In this paper, we compare the performance of several parallel and serial methods for solving dense real symmetric eigensystems on a distributed memory message passing parallel computer. We focus on matrices of sizeN=200 and processor countsP=1 toP=512, with execution on the Intel Touchstone DELTA computer. The best eigensolver method is found to depend on the number of available processors. Of the methods tested, a recently developed Blocked Factored Jacobi (BFJ) method is the slowest for smallP, but the fastest for largeP. Its speed is a complicated non-monotonic function of the number of processors used. A detailed performance analysis of the BFJ method shows that: (1) the factor most responsible for limited speedup is communication startup cost; (2) with current communication costs, the maximum achievable parallel speedup is modest (one order of magnitude) compared to the best serial method; and (3) the fastest solution is often achieved by using less than the maximum number of available processors.Pacific Northwest Laboratory is operated for the U.S. Department of Energy (DOE) by Battelle Memorial Institute under contract DE-AC06-76RLO 1830     

A semi-automated remotely operated system for manipulation of radioactive gases

A remote and semi-automated system for hot cell processing of accelerator produced radioactive gases, such as¹²³Xe,⁷⁷Kr, and²¹¹Rn is described. Detailed construction plans and a listing of the mechanical and electronic components are provided.Research carried out at Brookhaven National Laboratory under contract with the U. S. Department of Energy and supported by its Office of Health and Environmental Research.     

Non-NAA bomb Detection

Research sponsored by the Office of Energy Research, U.S. Department of Energy, under contract DE-AC05-840R21400 with Martin Marietta Energy Systems, Inc.     

A critical examination of the salicylaldehyde method for the determination of primary amines in the presence of secondary amines

Summary The salicylaldehyde method for the differentiation of primary and secondary amines in mixtures has been critically evaluated. This method yields best results in acetonitrile. In mixtures of amines one can expect high results for the primary amine with correspondingly low results for the secondary amine. Corrections can be made with known mixtures of the amines.Work performed under the auspices of the U.S. Department of Energy by the Lawrence Livermore Laboratory under contract number W-7405-ENG-48.     

Parallel computation of the MP2 energy on distributed memory computers

A parallel distributed implementation of the second-order Møller-Plesset perturbation theory method, widely used in quantum chemistry, is presented. Parallelization strategy and performance for the HONDO quantum chemistry program running on a network of Unix computers are also discussed. Superlinear speedups are obtained through a combined use of the CPU and memory of the different processors. Performance for standard and direct algorithms are presented and discussed. A superdirect algorithm that eliminates the communication bottleneck during the integral transformation step is also proposed. © 1995 by John Wiley & Sons, Inc.     

Cyclotron isotopes and radiopharmaceuticals XXXI. Improvements in77Br production and radiochemical separation from enriched78Se+

An improved method for production of >100 mCi of⁷⁷Br with the⁷⁸Se(p, 2n)⁷⁷Br nuclear reaction and a 4π water-cooled target containing encapsulated metallic⁷⁸Se or a Pb⁷⁸Se alloy has been developed. The⁷⁷Br was separated with ∼98% radiochemical yield and a radionuclidic purity of 98.9%. The time required to isolate carrier-free⁷⁷Br free of metallic impurities was less than 4hrs. Isotopically enriched⁷⁸Se was quantitatively recovered. This research was partially supported by NIH Grant No. Ro1 H1 18487-01, and Performed at Brookhaven National Laboratory under contract with the U.S. Department of Energy and supported by its Division of Basic Energy Sciences.     

Melting of indium by temperature-modulated differential scanning calorimetry

The melting and crystallization of a sharply melting standard has been explored for the calibration of temperature-modulated differential scanning calorimetry, TMDSC. Modulated temperature and heat flow have been followed during melting and crystallization of indium. It is observed that indium does not supercool as long as crystal nuclei remain in the sample when analyzing quasi-isothermally with a small modulation amplitude. For standard differential scanning calorimetry, DSC, the melting and crystallization temperatures of indium are sufficiently different not to permit its use for calibration on cooling, unless special analysis modes are applied. For TMDSC with an underlying heating rate of 0.2 K min^–1 and a modulation amplitude of 0.5–1.5 K at periods of 30–90 s, the extrapolated onsets of melting and freezing were within 0.1 K of the known melting temperature of indium. Further work is needed to separate the effects originating from loss of steady state between sample and sensor on the one hand and from supercooling on the other.On leave from Toray Research Center, Inc., Otsu, Shiga 520, Japan.This work was supported by the Division of Materials Research, National Science Foundation, Polymers Program, Grant # DMR 90-00520 and the Division of Materials Sciences, Office of Basic Energy Sciences, U.S. Department of Energy at Oak Ridge National Laboratory, managed by Lockheed Martin Energy Research Corp. for the U.S. Department of Energy, under contract number DEACOS-960R22464. Support for instrumentation came from TA Instruments, Inc. and Mettler-Toledo Inc. Research support was also given by ICI Paints.     

Validation of NAA data for a background soils characterization project

Background soils from areas around the United States Department of Energy facilities in Oak Ridge, Tennessee were characterized as part of an environmental restoration project. The data obtained in this project were validated using guidelines from the Environmental Protection Agency (EPA) Contract Laboratory Program (CLP), when EPA methods were used. However, there are no final EPA guidelines for validation of data obtained using radiochemical analytical methods, so procedures for validation had to be developed. This paper will describe the validation guidelines that were developed for neutron activation analysis (NAA) data and discuss the regulatory basis for them.Managed by Martin Marietta Energy Systems, Inc. for the U.S. DEPARTMENT OF ENERGY under contract DE-AC05-84OR21400     

Radioactive fallout from the chernobyl nuclear reactor accident

Following the accident at the nuclear reactor at Chernobyl, in the Soviet Union on April 26, 1986, we performed a variety of measurements to determine the level of the radioactive fallout on the western United States. We used gamma-spectroscopy to analyze air filters from the areas around Lawrence Livermore National Laboratory (LLNL), California, and Barrow and Fairbanks, Alaska. Milk from California and imported vegetables were also analyzed. The levels of the various fission products detected were far below the maximum permissable concentration levels.Work performed under the auspices of the U.S. Department of Energy by the Lawrence Livermore National Laboratory under contract number W-7405-ENG-48.