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arXiv · 2601.12570

INTERFACE Force Field for Alumina with Validated Bulk Phases and a pH-Resolved Surface Model Database for Electrolyte and Organic Interfaces

Cheng Zhu·Krishan Kanhaiya·Samir Darouich·Sean P. Florez·Karnajit Sen·Patrick Keil·Nawel S. Khelfallah·Eduard Schreiner·Ratan K. Mishra·Hendrik Heinz
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Abstract

Alumina and aluminum oxyhydroxides underpin chemical-engineering technologies from heterogeneous catalysis, corrosion protection, functional coatings, energy-storage devices, to biomedical components. Yet molecular models that predictively connect phase structure, pH-dependent surface chemistry, electrolyte organization, and adsorption across operating conditions remain limited. Here we introduce a unified INTERFACE Force Field (IFF) parameterization together with a curated, ready-to-use pH-resolved surface model database that provides the most accurate and transferable atomistic description of major alumina phases to date. The framework covers a-Al2O3, g-Al2O3, boehmite, diaspore, and gibbsite using a single, physically interpretable parameter set that is directly compatible with CHARMM, AMBER, OPLS-AA, CVFF, and PCFF. Across structural, thermodynamic, mechanical, and interfacial benchmarks, simulations reproduce experimental reference data with more than 95 percent accuracy, exceeding existing force fields and the reliability of current density-functional approaches. A key advance is the first transferable treatment of surface ionization and charge regulation across alumina phases over a broad range of pH values, enabling simulations of realistic solid electrolyte interfaces without phase-specific reparameterization. Quantitative reliability is demonstrated by reproducing trends in zeta potentials and pH-dependent adsorption of a corrosion inhibitor at alumina-water interfaces. Predicted adsorption free energies and surface contact times correlate with experiments across more than an order of magnitude. Relative to ML-DFT workflows, the speed 100 to 1000 times faster, reaching system sizes and time scales inaccessible to quantum methods. The results establish a predictive computational platform to design alumina-containing functional materials under realistic process conditions.

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Cheng Zhu, Krishan Kanhaiya, Samir Darouich, Sean P. Florez, Karnajit Sen, Patrick Keil, Nawel S. Khelfallah, Eduard Schreiner, Ratan K. Mishra, Hendrik Heinz. 2026-01-18. INTERFACE Force Field for Alumina with Validated Bulk Phases and a pH-Resolved Surface Model Database for Electrolyte and Organic Interfaces. https://arxiv.org/abs/2601.12570

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