{"doi":"10.1063/5.0296997","title":"How accurate are DFT forces? Unexpectedly large uncertainties in molecular datasets","abstract":"<jats:p>Training of general-purpose machine learning interatomic potentials (MLIPs) relies on large datasets with properties usually computed with density functional theory (DFT). A prerequisite for accurate MLIPs is that the DFT data are well converged to minimize numerical errors. A possible symptom of errors in DFT force components is nonzero net force. Here, we consider net forces in datasets including SPICE, Transition1x, ANI-1x, ANI-1xbb, AIMNet2, QCML, and OMol25. Several of these datasets suffer from significant nonzero DFT net forces. We also quantify individual force component errors by comparison to recomputed forces using more reliable DFT settings at the same level of theory, and we find significant discrepancies in force components averaging from 1.7 meV/Å in the SPICE dataset to 33.2 meV/Å in the ANI-1x dataset. These findings underscore the importance of well converged DFT data as increasingly accurate MLIP architectures become available.</jats:p>","journal":"The Journal of Chemical Physics","year":2025,"id":654622,"datarank":0.31191623125197543,"base_score":2.0794415416798357,"endowment":2.0794415416798357,"self_citation_contribution":0.31191623125197543,"citation_network_contribution":0.0,"self_endowment_contribution":0.31191623125197543,"citer_contribution":0.0,"corpus_percentile":null,"corpus_rank":null,"citation_count":7,"citer_count":0,"citers_with_citation_signal":0,"citers_with_endowment":0,"datacite_reuse_total":0,"is_dataset":false,"is_dataset_confidence":null,"is_data_producer":false,"deposit_databanks":null,"is_oa":false,"file_count":0,"downloads":0,"has_version_chain":false,"published_date":null,"fair_score":null,"fair_percentile":null,"algorithm_id":"datarank_citation_only_1hop_v6","ranking_scope":"data_only","authors":[{"id":1708471,"name":"Fabian Berger","orcid":"0000-0002-5463-3159","position":1,"is_corresponding":false},{"id":355756,"name":"Gábor Csányi","orcid":"0000-0002-4429-3031","position":2,"is_corresponding":false},{"id":1708472,"name":"Angelos Michaelides","orcid":"0000-0002-9169-169X","position":3,"is_corresponding":false},{"id":1708470,"name":"Domantas Kuryla","orcid":"0009-0001-2369-3693","position":0,"is_corresponding":false}],"reference_count":0,"raw_metadata":{"has_enrichment":true,"resolved":true,"title":"How accurate are DFT forces? Unexpectedly large uncertainties in molecular datasets","abstract":"<jats:p>Training of general-purpose machine learning interatomic potentials (MLIPs) relies on large datasets with properties usually computed with density functional theory (DFT). A prerequisite for accurate MLIPs is that the DFT data are well converged to minimize numerical errors. A possible symptom of errors in DFT force components is nonzero net force. Here, we consider net forces in datasets including SPICE, Transition1x, ANI-1x, ANI-1xbb, AIMNet2, QCML, and OMol25. Several of these datasets suffer from significant nonzero DFT net forces. We also quantify individual force component errors by comparison to recomputed forces using more reliable DFT settings at the same level of theory, and we find significant discrepancies in force components averaging from 1.7 meV/Å in the SPICE dataset to 33.2 meV/Å in the ANI-1x dataset. These findings underscore the importance of well converged DFT data as increasingly accurate MLIP architectures become available.</jats:p>","is_dataset_classified":null,"base_score":1.791759469228055,"endowment":1.791759469228055,"datacite_reuse_total":0,"file_count":0,"downloads":0,"views":0,"has_version_chain":false,"is_dataset":false,"is_oa":false,"pmid":"41369061","pmcid":null,"openalex_id":"https://openalex.org/W4417189401","authors":[],"funders":[{"funder_name":"EPSRC Center for Doctoral Training in Automated Chemical Synthesis Enabled by Digital Molecular Technologies","grant_id":"EP/S024220/1","title":null},{"funder_name":"n-AQUA","grant_id":"101071937","title":null},{"funder_name":"Materials Chemistry HEC Consortium","grant_id":"EP/X035859/1","title":null},{"funder_name":"High End Computing Materials Chemistry Consortium","grant_id":"EP/R029431/1","title":null},{"funder_name":"Cambridge Service for Data Driven Discovery","grant_id":"EP/T022159/1","title":null},{"funder_name":"DiRAC","grant_id":"","title":null}],"total_grants":6,"fwci":1.3253,"citation_percentile":0.80504132,"influential_citations":0,"citation_trend":[{"year":2026,"count":5}],"oa_status":"hybrid","license":"cc-by","oa_locations":[{"url":"https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/5.0296997/20833878/224313_1_5.0296997.pdf","host_type":"journal"},{"url":"https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/5.0296997/20833878/224313_1_5.0296997.pdf","host_type":"publisher"},{"url":"https://doi.org/10.1063/5.0296997","host_type":"journal"},{"url":"https://pubmed.ncbi.nlm.nih.gov/41369061","host_type":"repository"}],"fields_of_study":["Machine Learning in Materials Science","Computational Drug Discovery Methods","Advanced Physical and Chemical Molecular Interactions"],"mesh_terms":[],"keywords":["Density functional theory","Component (thermodynamics)","Training set","Interatomic potential","Net (polyhedron)","Data modeling"],"sdg_mappings":[],"linked_datasets":[],"clinical_trials":[],"software_tools":[],"database_accessions":[],"source":"live","citation_network_status":"fetched"},"created_at":"2026-08-11T07:33:57.675906Z","pmid":null,"pmcid":null,"fwci":null,"citation_percentile":null,"influential_citations":0,"oa_status":null,"license":null,"views":0,"total_file_size_bytes":0,"version_count":0,"fair_f":null,"fair_a":null,"fair_i":null,"fair_r":null,"fair_zscore":null,"fair_rationale":null,"fair_model":null,"fair_agent_version":null,"fair_fulltext_source":null,"fair_has_llm":null,"fair_computed_at":null,"clinical_trials":[],"software_tools":[],"db_accessions":[],"linked_datasets":[],"topics":[]}