Systematic over-binding in ZAFF-AMBER absolute binding free energy calculations for zinc-metalloenzyme inhibitors: a 14-compound accuracy benchmark on MMP-1

Absolute binding free energy (ABFE) calculation on zinc metalloenzymes stress-tests fixed-charge zinc force fields such as ZAFF-AMBER. We benchmark the ZAFF-AMBER + GAFF-2 + AM1-BCC ABFE protocol against experimental affinity for fourteen MMP-1 inhibitors drawn from PubChem bioassay records (IC50 0.78 nM to 98 µM; eleven hydroxamates, two carboxylates, one phosphonate), each carrying its PubChem CID, assay AID and retrieval timestamp. The protocol over-binds every compound, by 0.6 to 58.1 kcal/mol, and the over-binding is governed by the chelation strength of the warhead rather than by the measured potency: a weak (50 µM) hydroxamate still over-binds by 43 kcal/mol while a mid-potency (77 nM) phosphonate over-binds by only 4 kcal/mol. The rank correlation is weak and imprecise (Spearman 0.587, 95% CI [0.041, 0.847]; Pearson 0.631) with no sign-flips. Within-run statistical precision (0.5 to 0.9 kcal/mol) is not accuracy. We also document two pipeline failure modes and their fixes (a ReplicaExchangeSampler swap-all deadlock, and a production NaN crash requiring an explicit warmup) and contrast ABFE single-compound instability with population-level xtb rank stability. We recommend that fixed-charge ZAFF-AMBER ABFE not be used to rank zinc-chelating metalloenzyme inhibitors without warhead-stratified error budgeting. All data, code and provenance are attached and released at https://github.com/crazat/genesis_medicine (Apache-2.0). Provenance note: this is a fresh accuracy benchmark on a real, PubChem-sourced panel. An earlier draft of this work used a fabricated calibration panel and was withdrawn before any deposit; none of its compound identities, potencies or accuracy claims are carried into this record.

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Publication Details

Journal
Zenodo (CERN European Organization for Nuclear Research)
Published
2026-07-23
DOI
https://doi.org/10.5281/zenodo.21511724
Primary Topic
Protease and Inhibitor Mechanisms
Type
preprint
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preprint

Systematic over-binding in ZAFF-AMBER absolute binding free energy calculations for zinc-metalloenzyme inhibitors: a 14-compound accuracy benchmark on MMP-1

Cheongwoo Han
Zenodo (CERN European Organization for Nuclear Research)
Protease and Inhibitor Mechanisms
preprint

Systematic over-binding in ZAFF-AMBER absolute binding free energy calculations for zinc-metalloenzyme inhibitors: a 14-compound accuracy benchmark on MMP-1

Cheongwoo Han
preprint en

Abstract

Absolute binding free energy (ABFE) calculation on zinc metalloenzymes stress-tests fixed-charge zinc force fields such as ZAFF-AMBER. We benchmark the ZAFF-AMBER + GAFF-2 + AM1-BCC ABFE protocol against experimental affinity for fourteen MMP-1 inhibitors drawn from PubChem bioassay records (IC50 0.78 nM to 98 µM; eleven hydroxamates, two carboxylates, one phosphonate), each carrying its PubChem CID, assay AID and retrieval timestamp. The protocol over-binds every compound, by 0.6 to 58.1 kcal/mol, and the over-binding is governed by the chelation strength of the warhead rather than by the measured potency: a weak (50 µM) hydroxamate still over-binds by 43 kcal/mol while a mid-potency (77 nM) phosphonate over-binds by only 4 kcal/mol. The rank correlation is weak and imprecise (Spearman 0.587, 95% CI [0.041, 0.847]; Pearson 0.631) with no sign-flips. Within-run statistical precision (0.5 to 0.9 kcal/mol) is not accuracy. We also document two pipeline failure modes and their fixes (a ReplicaExchangeSampler swap-all deadlock, and a production NaN crash requiring an explicit warmup) and contrast ABFE single-compound instability with population-level xtb rank stability. We recommend that fixed-charge ZAFF-AMBER ABFE not be used to rank zinc-chelating metalloenzyme inhibitors without warhead-stratified error budgeting. All data, code and provenance are attached and released at https://github.com/crazat/genesis_medicine (Apache-2.0). Provenance note: this is a fresh accuracy benchmark on a real, PubChem-sourced panel. An earlier draft of this work used a fabricated calibration panel and was withdrawn before any deposit; none of its compound identities, potencies or accuracy claims are carried into this record.

Zenodo (CERN European Organization for Nuclear Research)
Genesis Medical Center (US)
Affordable and clean energy
Protease and Inhibitor Mechanisms
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