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arxiv: 2503.17124 · v1 · pith:3GL4AOLXnew · submitted 2025-03-21 · ❄️ cond-mat.mtrl-sci · cond-mat.supr-con

High-throughput study of kagome compounds in the AV3Sb5 family

Thalis H. B. da Silva , Tiago F. T. Cerqueira , Hai-Chen Wang , Miguel A. L. Marques This is my paper

Pith reviewed 2026-05-22 23:07 UTC · model grok-4.3

classification ❄️ cond-mat.mtrl-sci cond-mat.supr-con
keywords kagome compoundsAV3Sb5high-throughput DFTthermodynamic stabilityelectronic propertiesDirac pointsVan Hove singularitiesflat bands
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The pith

Atomic substitutions in AV3Sb5 yield 36 thermodynamically stable kagome compounds including with Au, Hg, Tl and Ce.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The paper applies machine-learning-accelerated density functional theory to scan atomic substitutions across the AV3Sb5 kagome structure. It locates 36 new candidates that lie on the convex hull of thermodynamic stability, plus many others nearby. Stable examples appear not only when the C site holds a pnictogen but also when it holds Au, Hg, Tl or Ce. Several of these materials display Dirac points, Van Hove singularities or flat bands near the Fermi level. The expanded chemistry therefore supplies fresh platforms for tuning superconductivity and topological behavior in kagome lattices.

Core claim

By performing machine-learning-accelerated high-throughput density functional theory calculations on atomic substitutions in the AV3Sb5 structure, we identify 36 promising candidates that are thermodynamically stable, with many more close to the convex hull. Stable compounds are not only found with a pnictogen (Sb or Bi) as the C atom but also with Au, Hg, Tl, and Ce. This diverse chemistry opens the way to tune the electronic properties of the compounds. In fact, many of these compounds exhibit Dirac points, Van Hove singularities, or flat bands close to the Fermi level.

What carries the argument

Machine-learning-accelerated high-throughput density functional theory calculations that evaluate formation energies and convex-hull distances for substituted AB3C5 kagome structures.

If this is right

  • The 36 stable compounds become concrete targets for experimental synthesis and measurement of superconductivity or charge-density-wave order.
  • Substitution with Au, Hg, Tl or Ce provides chemical knobs to shift Dirac points, Van Hove singularities and flat bands relative to the Fermi level.
  • Compounds lying close to the convex hull may become accessible through modest pressure, temperature or doping adjustments.
  • The same screening workflow can be reused on other kagome parent structures to enlarge the known material set.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

  • The newly identified flat-band compounds are natural candidates for follow-up many-body calculations that search for correlated phases beyond single-particle DFT.
  • Because the parent AV3Sb5 materials already show charge-density waves, the substituted variants offer a systematic route to map how C-site chemistry controls the wave-vector and gap size.
  • Close-to-hull compounds that remain metastable could be realized as thin films or under epitaxial strain, testable by targeted growth experiments.

Load-bearing premise

The chosen exchange-correlation functional and pseudopotentials produce formation energies accurate enough to identify true ground-state compounds among the substitutions.

What would settle it

Laboratory synthesis of any one of the 36 predicted stable compounds followed by experimental measurement of its decomposition enthalpy or temperature would confirm or refute the calculated stability ranking.

Figures

Figures reproduced from arXiv: 2503.17124 by Hai-Chen Wang, Miguel A. L. Marques, Thalis H. B. da Silva, Tiago F. T. Cerqueira.

Figure 1
Figure 1. Figure 1: FIG. 1. Illustration of the kagome structure, showing both [PITH_FULL_IMAGE:figures/full_fig_p002_1.png] view at source ↗
Figure 2
Figure 2. Figure 2: FIG. 2. Distance above the convex hull (meV/atom) for candidate kagome compounds with composition [PITH_FULL_IMAGE:figures/full_fig_p003_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: FIG. 3. Stability profile of kagome compounds containing a [PITH_FULL_IMAGE:figures/full_fig_p004_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: FIG. 4. Electronic band structures of six newly proposed compounds. The black curve represents the total density of states [PITH_FULL_IMAGE:figures/full_fig_p005_4.png] view at source ↗
Figure 2
Figure 2. Figure 2: FIG. 2 [PITH_FULL_IMAGE:figures/full_fig_p017_2.png] view at source ↗
read the original abstract

The kagome lattice has emerged as a fertile ground for exotic quantum phenomena, including superconductivity, charge density waves, and topologically nontrivial states. While AV3Sb5 (A = K, Rb, Cs) compounds have been extensively studied in this context, the broader AB3C5 family remains largely unexplored. In this work, we employ machine-learning-accelerated, high-throughput density functional theory calculations to systematically investigate the stability and electronic properties of kagome materials derived from atomic substitutions in the AV3Sb5 structure. We identify 36 promising candidates that are thermodynamically stable, with many more close to the convex hull. Stable compounds are not only found with a pnictogen (Sb or Bi) as the C atom but also with Au, Hg, Tl, and Ce. This diverse chemistry opens the way to tune the electronic properties of the compounds. In fact, many of these compounds exhibit Dirac points, Van Hove singularities, or flat bands close to the Fermi level. Our findings provide an array of compounds for experimental synthesis and further theoretical exploration of kagome superconductors beyond the already known systems.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Referee Report

1 major / 1 minor

Summary. The paper employs machine-learning-accelerated high-throughput DFT to screen substitutions in the AV3Sb5 kagome structure, identifying 36 thermodynamically stable AB3C5 compounds (including with C = Au, Hg, Tl, Ce) that lie on or near the convex hull, along with electronic features such as Dirac points, Van Hove singularities, and flat bands near the Fermi level.

Significance. If the stability rankings hold, the work substantially enlarges the known chemical space of kagome materials beyond the three established pnictogen-based parents, supplying a concrete list of candidates for synthesis and further study of superconductivity and topological states.

major comments (1)
  1. [Abstract and computational methods] Abstract and computational methods: the central claim of 36 thermodynamically stable candidates (including non-pnictogen C atoms) rests on ML-accelerated DFT formation energies correctly determining convex-hull placement, yet the manuscript reports neither benchmarking against the known AV3Sb5 parents, experimental formation energies, nor error estimates for the chosen functional/pseudopotentials, particularly for heavy elements where self-interaction or relativistic effects may exceed typical ~50 meV/atom thresholds.
minor comments (1)
  1. [Abstract] The abstract states 'many more close to the convex hull' without specifying the energy window or providing a quantitative distribution of distances to the hull.

Simulated Author's Rebuttal

1 responses · 0 unresolved

We thank the referee for their careful reading of the manuscript and for highlighting the need for explicit validation of the computational methodology. We address the single major comment below and will incorporate the requested information in a revised version.

read point-by-point responses

  1. Referee: [Abstract and computational methods] Abstract and computational methods: the central claim of 36 thermodynamically stable candidates (including non-pnictogen C atoms) rests on ML-accelerated DFT formation energies correctly determining convex-hull placement, yet the manuscript reports neither benchmarking against the known AV3Sb5 parents, experimental formation energies, nor error estimates for the chosen functional/pseudopotentials, particularly for heavy elements where self-interaction or relativistic effects may exceed typical ~50 meV/atom thresholds.

    Authors: We agree that the absence of explicit benchmarking and error quantification is a limitation of the current manuscript. In the revision we will add a new subsection under Computational Methods that (i) reports formation energies computed for the three established parents (KV3Sb5, RbV3Sb5, CsV3Sb5) and compares them to the limited available experimental data, (ii) quantifies the mean absolute error of the ML model on a held-out test set drawn from the same chemical space, and (iii) provides an estimate of the typical DFT error (~40–60 meV/atom) for the PBE functional with the employed pseudopotentials. For the heavy-element substitutions (Au, Hg, Tl, Ce) we have already employed scalar-relativistic pseudopotentials; we will explicitly note this choice and discuss the residual uncertainty associated with spin-orbit coupling and self-interaction. Because the screening relies on relative rather than absolute formation energies within a fixed chemical space, the convex-hull rankings remain informative even with these uncertainties, but we accept that the manuscript should make this caveat and the supporting numbers transparent. revision: yes

Circularity Check

0 steps flagged

No circularity in high-throughput DFT screening of kagome compounds

full rationale

The paper applies standard ML-accelerated DFT to compute formation energies and convex-hull stability for atomic substitutions in the AV3Sb5 structure. No load-bearing step reduces by construction to a fitted parameter, self-citation chain, or self-definitional ansatz; stability rankings are obtained from first-principles energies compared against external elemental references. The workflow is self-contained against independent benchmarks (known parent compounds, convex-hull construction) and does not rename empirical patterns or smuggle assumptions via prior author work.

Axiom & Free-Parameter Ledger

0 free parameters · 1 axioms · 0 invented entities

The central claim rests on the domain assumption that standard DFT formation energies correctly identify thermodynamic stability for these intermetallic compounds and that the kagome structure type is preserved under substitution.

axioms (1)
  • domain assumption Density functional theory with typical approximations yields formation energies accurate enough to determine thermodynamic stability and proximity to the convex hull.
    Invoked throughout the high-throughput screening described in the abstract.

pith-pipeline@v0.9.0 · 5753 in / 1169 out tokens · 56215 ms · 2026-05-22T23:07:16.566418+00:00 · methodology

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Reference graph

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