This multi-institutional program, led by Sandia National Laboratories, creates a computational framework to accelerate discovery and characterization of complex molecular systems targeting gas-phase and coupled heterogeneous/gas-phase reactions and mechanisms with relevance to catalysis. The work involves modern theoretical chemistry combined with improved mathematical software for solving complex problems on exascale-size supercomputers, aiming to develop a uniquely powerful chemical computational toolset for the research community.
Argonne National Laboratory’s role in this effort is to create a modern, intelligent, user-friendly, and accurate thermodynamic database that is self-consistent and can be accessed and grown by the broader scientific community. For gas-phase systems, this effort will incorporate automatic state-of-the-art energy evaluations, including pertinent anharmonic corrections, and generate thermochemical and thermophysical properties directly applicable in common kinetics codes.
In particular, the goal of the program is to create an accessible scientific database that gives collaborators direct access to the Active Thermochemical Tables (ATcT), allowing it to greatly expand its focus. The program will help generalize ATcT to all thermochemistry fields, including materials science, atmospheric chemistry, and condensed phase chemistry, and will improve the results of thermochemistry-dependent models in those fields. This work will also improve the mechanisms by which thermodynamic information is validated, used, and presented, such that the entire community at large can utilize the best currently available information.
Argonne National Laboratory is home of a current petascale computational resource (Theta) and an upcoming exascale resource (Aurora). The effort at Argonne National Laboratory includes direct collaboration with computer scientists at the ALCF (Argonne Leadership Computing Facility) to ensure that the frameworks developed under these efforts run at scale, primarily through an Early Science Program led by Argonne.
- D. H. Bross, A. W. Jasper, B. Ruscic, and A. F. Wagner. Toward Accurate High Temperature Anharmonic Partition Functions. Proc. Combust. Inst. 37, 315-322 (2019)
- B. K. Welch, R. Dawes, D. H. Bross, B. Ruscic. An Automated Thermochemistry Protocol Based on Explicitly Correlated Coupled-Cluster Theory: The Methyl and Ethyl Peroxy Families. J. Phys. Chem. A 123, 5673-5682 (2019)
- T. L. Nguyen, J. H. Thorpe, D. H. Bross, B. Ruscic, and J. F. Stanton. Unimolecular Reaction of Methyl Isocyanide to Acetonitrile: A High-Level Theoretical Study. J. Phys. Chem. Lett. 9, 2532–2538 (2018)
- D. H. Bross, H.-G. Yu, L. B. Harding, and B. Ruscic. Active Thermochemical Tables: The Partition Function of Hydroxymethyl (CH2OH) Revisited, J. Phys. Chem. A 123, 4212-4231 (2019)
- B. Ruscic and D. H. Bross, Thermochemistry, Computer-Aided Chem. Eng. 45, 3-114 (2019) [a.k.a. Ch. 1 in: Mathematical Modeling of Complex Reaction Systems: Pyrolysis and Combustion, T. Faravelli, F. Manenti, and E. M. Ranzi, Eds., Computer Aided Chemical Engineering Series, Vol. 45, Elsevier: New York, NY, 2019, pp. 3-114]
- D. Feller, D. H. Bross, and B. Ruscic. Enthalpy of Formation of C2H2O4 (Oxalic Acid) from High-Level Calculations and the Active Thermochemical Tables Approach, J. Phys. Chem. A 123, 3481-3496 (2019)
- J. H. Thorpe, C. A. Lopez, T. L. Nguyen, J. H. Baraban, D. H. Bross, B. Ruscic, and J. F. Stanton. High-Accuracy Extrapolated ab initio Thermochemistry. IV. A Modified Recipe for Computational Efficiency, J. Chem. Phys. 150, 224102/1-224102/16 (2019)