{"id":"f24de0a8-92ff-44ca-a188-3dc781f4c461","arxiv_id":"2504.20812","paper_version":1,"verdict":"ACCEPT","confidence":"HIGH","novelty_score":6.0,"correctness_risk":"medium","formal_verification":"none","parameter_count":1,"one_line_summary":"An open database of 7,024 inorganic materials computed with all-electron HSE06 hybrid DFT, including stability metrics and a SISSO model for HSE06 band gaps.","lead":"Researchers built an open database of 7,024 inorganic materials using all-electron hybrid functional DFT calculations, going beyond the usual GGA accuracy. The database includes band gaps, formation energies, and decomposition energies from convex hull and Pourbaix diagrams, and is shown to be usable for training interpretable AI models.","discovery_kind":"new_application","skeptic_critique":{"model":"deepseek-v4-flash","headline":"PBEsol-geometry single-point assumption is the main risk: near-hull stability and Pourbaix classifications can flip under HSE06 relaxation, and the paper's own examples show meV-scale flips.","rationale":"I agree with the reader that PBEsol geometries are the weakest link, and I sharpen it with an energy-scale argument: near-hull classifications are decided on the 4-50 meV/atom scale, which is exactly the scale on which single-point versus relaxed hybrid geometries can act. This is a genuine soft spot, but it does not overturn acceptance. The paper is transparent about the approximation, cites prior evidence that HSE06 changes lattice constants only slightly, provides open data and scripts, and benchmarks band gaps against experiment (MAE 0.62 eV, about 50% better than PBEsol). The database's primary value is the openly available all-electron HSE06 energies and derived tabulated properties; even if a small fraction of near-hull stability labels shift under HSE06 relaxation, the dataset remains useful for training and screening, and the limitation is disclosed in the final limitations paragraph. A targeted HSE06-relaxation validation would strengthen the stability claims, so I would keep the reader's ACCEPT verdict unchanged rather than making acceptance conditional.","tokens_in":7783,"tokens_out":9556,"duration_ms":107827,"concrete_test":"Identify all materials with |Delta Hd,HSE06| <= 50 meV/atom and all with |Delta G_pbx,HSE06| <= 0.1 eV/atom. Re-relax this subset with HSE06 in FHI-aims using the same basis and convergence settings, recompute decomposition energies from the convex hull and Pourbaix diagrams, and count how many materials cross the 50 meV/atom or 0.1 eV/atom thresholds. Report the mean and maximum energy change per atom. If the flip rate is a few percent and mean shifts are below 10 meV/atom, the single-point approximation is adequate for screening; if flips are frequent or shifts exceed 25 meV/atom, the stability metrics should be reported as PBEsol-geometry/HSE06-energy estimates rather than full HSE06 predictions.","verdict_should_be":"UNCHANGED","load_bearing_attack":"The central stability claims inherit the PBEsol-geometry approximation. Section II states HSE06 energies are evaluated on PBEsol-optimized structures, and Section IV uses these values to build convex hull phase diagrams and Pourbaix diagrams. The relevant error is not average lattice-constant agreement but the shift in relative energies between PBEsol and HSE06 geometries. The paper's own examples are concerning: Li2Al is stable by PBEsol and unstable by 4 meV/atom with HSE06; Co(PtO3)2 flips in the opposite direction by 11 meV/atom. The acid-stability criterion is 0.1 eV/atom and the Delta G_pbx MAD between PBEsol and HSE06 is 0.27 eV/atom, so the protocol operates in a regime where geometry-induced shifts of tens of meV/atom can change classifications. The limitations paragraph acknowledges HSE06-relaxed geometries may be needed for defects and band edge alignments, but it does not test whether stability metrics are sensitive. Without such a test, the database's stability labels are HSE06 energetics projected onto PBEsol geometries, and the magnitude of the projection error is unknown.","agreement_with_reader":"agree"},"referee_report":{"model":"deepseek-v4-flash","summary":"This paper presents a database of 7,024 inorganic materials with all-electron hybrid functional (HSE06) total energies, band gaps, formation energies, and stability metrics, computed on PBEsol-relaxed geometries using FHI-aims. The authors construct convex hull and Pourbaix diagrams for stability analysis, and demonstrate a SISSO-based machine-learning model for HSE06 band gaps. The database is made publicly available through NOMAD and figshare.","tokens_in":7965,"tokens_out":4492,"duration_ms":41964,"significance":"The database is a valuable open resource that extends hybrid-functional accuracy to a broad chemical space using an all-electron approach, with publicly accessible data repos and a transparent workflow. The band-gap benchmarking against experiment (MAE 0.62 eV for HSE06 vs 1.35 eV for PBEsol on 121 materials) provides concrete evidence of improved electronic property prediction. The interpretable SISSO model with nested cross-validation is a useful illustration of how the database can support AI models. If the geometry-sensitivity concern is addressed, the database and its stability metrics would be a strong community resource.","major_comments":[{"comment":"The central stability claims rely on HSE06 single-point energies evaluated on PBEsol-relaxed geometries. The paper's own examples show that differences between PBEsol and HSE06 at fixed geometry can flip stability classifications (e.g., Li2Al is stable with PBEsol but unstable by 4 meV/atom with HSE06; Co(PtO3)2 is unstable by 11 meV/atom with PBEsol but stable with HSE06). However, these examples do not quantify the effect of geometry relaxation, and the argument based on lattice-constant accuracy does not directly address relative energy shifts. Since the acid-stability criterion is 0.1 eV/atom and the PBEsol–HSE06 MAD for Pourbaix decomposition energies is 0.27 eV/atom, geometry-induced shifts of tens of meV/atom could change stability assignments. The authors should perform HSE06 relaxation for a representative subset of near-hull and Pourbaix-relevant materials and report how many stability classifications change. Without this test, the stability labels are HSE06 energetics projected onto PBEsol geometries, and the magnitude of the projection error is unknown.","section":"Section IV, convex hull and Pourbaix analysis"}],"minor_comments":[{"comment":"Typographical errors: \"he data\" should be \"the data\", and \"Crystral\" should be \"Crystal\" in \"Inorganic Crystral Structure Database\".","section":"Section II"},{"comment":"The word \"Distriution\" should be \"Distribution\".","section":"Fig. 7 caption"},{"comment":"The statement \"A MAD of 0.27 eV/atom is observed between the two methods\" for Pourbaix decomposition energies would benefit from explicit clarification that this is the mean absolute deviation across all materials, as it can be misread as a per-reaction value.","section":"Section IV"},{"comment":"The equation uses the symbol \\langle NVAC\\rangle, but the text only defines \\langle NVAL\\rangle as the number of valence orbitals; please define NVAC and clarify the notation.","section":"Equation (1) and descriptor definitions"},{"comment":"The SISSO model uses the PBEsol band gap as a feature to predict the HSE06 band gap; stating explicitly that this is a delta-learning or correction approach would improve clarity.","section":"Section IV, SISSO model"}],"recommendation":"major_revision","confidential_remarks":"The paper is likely to be of interest to the broad community using DFT databases. The main concern is not about the data production but about the interpretation of stability metrics under the single-point geometry approximation; I recommend requiring a sensitivity test before publication. The authors' response to this point will determine whether the stability claims can stand."},"author_rebuttal":null,"desk_editor":{"model":"deepseek-v4-flash","letter":"Colleague,\n\nThis paper is worth a serious look. It introduces a database of 7,024 materials with all-electron HSE06 total energies, band gaps, convex hull decomposition energies, and Pourbaix decomposition energies, all made available through NOMAD and figshare. That combination—all-electron hybrid-functional data plus stability metrics—is new to my knowledge. The authors also demonstrate a SISSO model for HSE06 band gaps as an example of the database's utility.\n\nWhat the paper does well: the workflow is clearly described, the data are public, and the band gap benchmark against experiment shows the expected improvement (MAE from 1.35 eV with PBEsol to 0.62 eV with HSE06 on 121 materials). The limitations are honestly stated: PBEsol geometries, no temperature/pressure effects, and the 198 non-converged materials are all disclosed up front.\n\nThe main soft spot is the PBEsol-geometry single-point approximation for HSE06 energies. The paper justifies it by citing small lattice constant differences, but the property that matters for stability is relative energies, not absolute lattice constants. The paper's own examples show that switching from PBEsol to HSE06 energies at the same geometry flips Li2Al by 4 meV/atom and Co(PtO3)2 by 11 meV/atom. The MAD between PBEsol and HSE06 Pourbaix decomposition energies is 0.27 eV/atom, large relative to the 0.1 eV/atom acid-stability threshold. The authors acknowledge HSE06-relaxed geometries might be needed for defects and band edge alignments, but they do not test whether stability classifications themselves are sensitive to geometry. That is a legitimate concern, and a handful of HSE06 re-optimizations for near-hull phases would settle it. It is not a fatal flaw—these are energy shifts of tens of meV, and the database will still serve many purposes—but the stability labels should be treated as approximate.\n\nMinor quibbles: formation energies are not benchmarked against experiment, and the ICSD/MP-based selection may bias toward well-characterized structures. Neither is disqualifying.\n\nOverall, this is a solid data-resource contribution. I would send it to referees rather than desk reject, and I expect the geometry question to be the main point of debate. I'd also bring it to our reading group.\n\nBest,","headline":"A genuinely useful all-electron HSE06 database with stability metrics; the PBEsol-geometry single-point approximation is a real but acknowledged limitation that deserves scrutiny, not rejection.","tokens_in":8546,"tokens_out":3114,"would_cite":true,"duration_ms":31093,"reading_group":"yes","serious_thinker":"yes","would_accept_peer_review":true},"rs_alignment":null,"lean_confirmation":null,"pith_extraction":{"msc":[],"pacs":["71.15.Mb","71.20.-b"],"model":"deepseek-v4-flash","headline":"The paper constructs a database of 7,024 inorganic materials with all-electron hybrid-functional (HSE06) total energies and uses it to assess thermodynamic and electrochemical stability and to train interpretable AI models for band gaps.","keywords":["materials database","hybrid functional","HSE06","all-electron DFT","thermodynamic stability","Pourbaix diagram","band gap prediction","SISSO"],"falsifier":"Take a sample of roughly 50 oxides from the database, fully relax them with HSE06, and recompute their convex-hull and Pourbaix decomposition energies; if many materials change stable/unstable classification or decomposition energies shift by more than about 0.1 eV/atom, the single-point-on-PBEsol assumption is the weak link. An experimental check would compare the database's acid-stability predictions for the reported oxide set against measured dissolution or corrosion behavior at pH 0 and 1.23 V.","tokens_in":7527,"feed_emoji":"⚛️","tokens_out":11336,"duration_ms":100591,"temperature":0.7,"pith_summary":"Most materials databases rely on GGA functionals, which misjudge localized electronic states in transition-metal oxides and underestimate band gaps. This paper presents an open database of 7,024 inorganic materials computed with the all-electron, range-separated hybrid functional HSE06, alongside the PBEsol results used for geometries. For each material the database reports total energies, band gaps, formation energies, decomposition energies from convex hull phase diagrams, and Pourbaix decomposition energies at oxygen-evolution-reaction conditions (pH 0, U = 1.23 V). These data show systematic differences from GGA: HSE06 lowers formation energies, raises band gaps (experimental band-gap error drops from 1.35 eV to 0.62 eV), and flips some stability classifications, e.g. AgRhO2 is acid-stable at HSE06 but not with PBEsol. The authors also train a SISSO model on the database that predicts HSE06 band gaps, with 90% of errors within 7.5% of the dataset's band-gap spread.","feed_headline":"7,024 materials get hybrid-functional stability data","feed_subtitle":"All-electron HSE06 energies reveal which oxides survive acid OER conditions and train AI band-gap models.","key_machinery":"The central object is the database itself, produced by a two-stage workflow: geometry optimization with the PBEsol functional, chosen for accurate lattice constants, followed by single-point HSE06 energy and electronic-structure calculations, both performed all-electron with numerically atom-centered basis functions. HSE06 is a range-separated hybrid functional that mixes a fraction of exact exchange with semilocal exchange, correcting the band-gap underestimation of GGA functionals. Stability analysis is carried out by constructing convex hull phase diagrams and Pourbaix diagrams; the load-bearing quantities are the decomposition energies $\\Delta H_d$ and $\\Delta G^{\\mathrm{OER}}_{\\mathrm{pbx}}$, which turn total energies into statements about thermodynamic and acid electrochemical stability. The AI demonstration uses SISSO, a compressed-sensing symbolic-regression method, to find a compact descriptor for the HSE06 band gap.","core_discovery":"The paper sets out to establish that an openly accessible, all-electron hybrid-functional database can serve as a reliable basis for stability analysis and for training AI models for materials properties. The central results are a collection of 7,024 materials with HSE06 single-point energies on PBEsol-relaxed structures; quantitative stability metrics, namely the convex-hull decomposition energy $\\Delta H_d$ and the Pourbaix decomposition energy $\\Delta G^{\\mathrm{OER}}_{\\mathrm{pbx}}$, computed at both functional levels; and an interpretable SISSO descriptor that predicts HSE06 band gaps from PBEsol-computed features. The reported comparisons show a mean absolute deviation of 0.15 eV/atom between PBEsol and HSE06 formation energies, 0.77 eV for band gaps, and 0.27 eV/atom for Pourbaix decomposition energies; under the chosen criterion, 255 materials are acid-stable with HSE06 versus 222 with PBEsol. The paper presents examples where the two functionals identify different critical decomposition reactions and even reverse stability, such as AgRhO2.","pith_inferences":["Extending the workflow to full HSE06 geometry relaxation for a subset would quantify how much of the reported stability data depends on the PBEsol-geometry assumption; defect and band-edge properties are the most likely to be affected.","The Pourbaix analysis covers only pH 0 and U = 1.23 V; computing the full pH-potential grid for the acid-stable subset could reveal passivation or corrosion regimes that the current OER-focused criterion misses.","The SISSO descriptor includes the PBEsol band gap as an input feature, so its applicability to unexplored chemistries without a cheap band-gap estimate is an open question; retraining without that feature would test how much predictive power remains.","The same pipeline could be run with other reference structure sets or exchange-correlation functionals to build an ensemble of databases, giving a quantitative handle on how stability predictions depend on the initial structure filter."],"forward_implications":["AI models trained on this database inherit hybrid-functional accuracy for band gaps and stability, avoiding the systematic GGA errors that affect transition-metal oxides.","The database provides a concrete shortlist of acid-stable oxides for oxygen-evolution electrocatalysis: 255 materials satisfy the $\\Delta G^{\\mathrm{OER}}_{\\mathrm{pbx}} \\le 0.1$ eV/atom criterion at HSE06.","Functional choice matters for stability screening: PBEsol and HSE06 decomposition energies differ with a mean absolute deviation of 0.27 eV/atom for Pourbaix diagrams and can reverse individual stability classifications.","Because each material carries both PBEsol and HSE06 values, users can estimate functional-induced uncertainty in any property derived from the database.","The SISSO demonstration shows that HSE06 band gaps can be estimated from inexpensive PBEsol and composition features, with 90% of test errors within 7.5% of the band-gap spread in the dataset."],"supporting_citations":[{"why":"Provides the initial crystal structures and identifiers used to filter database entries.","marker":"[1]"},{"why":"Prior hybrid-functional band-gap database that motivates and contextualizes the HSE06 approach.","marker":"[11]"},{"why":"Prior high-throughput hybrid-functional calculations of band gaps and formation energies that this database extends.","marker":"[12]"},{"why":"Supplies the scalable all-electron implementation of hybrid functionals that makes 7,024 calculations feasible.","marker":"[15]"},{"why":"Provides the SISSO method used to build the interpretable band-gap descriptor model.","marker":"[16]"},{"why":"Defines the PBEsol functional used for geometry optimization of all structures.","marker":"[17]"},{"why":"Supports the use of hybrid functionals for formation energies and redox potentials of transition-metal compounds.","marker":"[19]"},{"why":"Supplies the experimental band-gap benchmark against which HSE06 reduces the mean absolute error to 0.62 eV.","marker":"[24]"},{"why":"Gives the scheme for combining first-principles solid energies with experimental aqueous species to construct Pourbaix diagrams.","marker":"[28]"}],"fun_headline_variants":["Hybrid DFT database: 7,024 materials for stability & AI","All-electron hybrid DFT unlocks 7,024 materials database","HSE06 database powers stability checks and AI models","7,024 materials with hybrid-functional energies for AI","New database: hybrid-functional energies for 7,024 solids"],"cache_read_input_tokens":3200,"weakest_assumption_plain":"The load-bearing premise is that PBEsol-relaxed geometries are close enough to HSE06 equilibrium geometries that single-point HSE06 energies give trustworthy relative stabilities; if the two functionals prefer different geometries for some oxide class, convex-hull and Pourbaix decomposition energies could shift and stability verdicts could flip.","fun_headline_variants_meta":{"raw":{"variants":["Hybrid DFT database: 7,024 materials for stability & AI","All-electron hybrid DFT unlocks 7,024 materials database","HSE06 database powers stability checks and AI models","7,024 materials with hybrid-functional energies for AI","New database: hybrid-functional energies for 7,024 solids"]},"model":"deepseek-v4-flash","effort":"low","cost_usd":0.001014,"raw_usage":{"total_tokens":4265,"prompt_tokens":908,"completion_tokens":3357,"prompt_tokens_details":{"cached_tokens":384},"prompt_cache_hit_tokens":384,"prompt_cache_miss_tokens":524,"completion_tokens_details":{"reasoning_tokens":3274}},"tokens_in":524,"tokens_out":3357,"duration_ms":21734,"temperature":1.0,"reasoning_tokens":3274,"cache_read_input_tokens":384,"cache_creation_input_tokens":0},"cache_creation_input_tokens":0},"created_at":"2026-08-16T05:18:50.250779+00:00","model_set":{"reader":"deepseek-v4-flash"},"falsifier":"Take a sample of roughly 50 oxides from the database, fully relax them with HSE06, and recompute their convex-hull and Pourbaix decomposition energies; if many materials change stable/unstable classification or decomposition energies shift by more than about 0.1 eV/atom, the single-point-on-PBEsol assumption is the weak link. An experimental check would compare the database's acid-stability predictions for the reported oxide set against measured dissolution or corrosion behavior at pH 0 and 1.23 V.","supporting_citations":[{"cited_title":null,"cited_arxiv_id":null,"evidence_quote":"Provides the initial crystal structures and identifiers used to filter database entries."},{"cited_title":null,"cited_arxiv_id":null,"evidence_quote":"Prior hybrid-functional band-gap database that motivates and contextualizes the HSE06 approach."},{"cited_title":null,"cited_arxiv_id":null,"evidence_quote":"Prior high-throughput hybrid-functional calculations of band gaps and formation energies that this database extends."},{"cited_title":"Kokott, F","cited_arxiv_id":null,"evidence_quote":"Supplies the scalable all-electron implementation of hybrid functionals that makes 7,024 calculations feasible."},{"cited_title":null,"cited_arxiv_id":null,"evidence_quote":"Supports the use of hybrid functionals for formation energies and redox potentials of transition-metal compounds."},{"cited_title":null,"cited_arxiv_id":null,"evidence_quote":"Gives the scheme for combining first-principles solid energies with experimental aqueous species to construct Pourbaix diagrams."}],"review_version":1}