2026-10-12T09:33:06Z https://api.figshare.com/v2/oai

oai:figshare.com:article/33911563 2026-09-17T20:37:46Z portal_1197 item_type_3 month_year_09_2026

Dataset for "Automated discovery of algorithms for molecular electronic structure calculations using physics-informed program synthesis" Kyle Acheson (15388816) Rastislav Turanyi (23496644) Scott Habershon (1263891) Migrated from ePrints We demonstrate a physics-informed program synthesis (PIPS) approach that can be used to identify entirely-new algorithms that approximate the results of single-reference electronic structure approaches like Hartree-Fock (HF) and density-functional theory (DFT) - but without any self-consistent field iterations at all. Our PIPS strategy exploits the fact that the eigenvectors of the Fock matrix F (or Kohn-Sham matrix K) are the same as the eigenvectors of a broad class of matrix functions, f(F). As a result, PIPS can be used to seek matrices M that yield the same molecular orbital coefficients as converged HF or DFT calculations. We demonstrate this approach by generating new algorithms that accurately predict total energies for a series of heterodiatomic molecules (LiCl, LiF, NaCl, NaF) and C1-C4 hydrocarbons; further simulations of C8-C20 alkane species demonstrate further transferability and efficiency of the resulting algorithms. We obtain novel algorithms that can reproduce HF or DFT energies to within 0.1 kcal/mol/atom while requiring only a single matrix-diagonalization operation, rather than an iterative self-consistent field convergence. The approach demonstrated here could be similarly applied to more complex wavefunction ansatze, opening an interesting optimization-based pathway to identifying accurate yet efficient algorithms for molecular quantum chemistry.<br><br>Supporting data for "Automated discovery of algorithms for molecular electronic structure calculations using physics-informed program synthesis”, including calculation data for diatomic molecules and alkane molecules. Both raw (unprocessed) and final (compiled) datasets are included. 2026-03-04T00:00:00Z Dataset Dataset 10.82444/warw.33911563.v1 https://figshare.com/articles/dataset/Dataset_for_Automated_discovery_of_algorithms_for_molecular_electronic_structure_calculations_using_physics-informed_program_synthesis_/33911563 CC BY 4.0