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SKM 2023 – wissenschaftliches Programm

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MM: Fachverband Metall- und Materialphysik

MM 36: Data Driven Materials Science: Big Data and Work Flows – Microstructure-Property-Relationships (joint session MM/CPP)

MM 36.9: Vortrag

Donnerstag, 30. März 2023, 12:30–12:45, SCH A 251

Efficient workflow for treating thermal and zero-point contributions to the formation enthalpies of ionic materials — •Rico Friedrich1,2,3, Marco Esters1, Corey Oses1, Stuart Ki1, Maxwell J. Brenner1, David Hicks1, Michael J. Mehl1, Cormac Toher1, and Stefano Curtarolo11Duke University, USA — 2TU Dresden — 3Helmholtz-Zentrum Dresden-Rossendorf

The formation enthalpy, quantifying the enthalpy of a compound with respect to its elemental references, is a key parameter for predicting the thermodynamic stability of materials thus enabling data-driven materials design. Although for instance zero-point vibrational and thermal contributions to the formation enthalpy can be quite substantial reaching absolute values of up to ∼50 meV/atom for ionic systems such as oxides, they are often neglected in ab initio workflows.

Here, we first calculate the thermal and zero-point contributions accurately from a quasi-harmonic Debye model. At room temperature, they largely cancel each other due to the different bond stiffness of compound and references reducing the total vibrational contribution to maximally ∼20 meV/atom [1]. Moreover, the vibrational contributions can be parametrized within the coordination corrected enthalpies (CCE) method completely eliminating the need to compute these terms explicitly. On this basis, using only 0 K ab initio data as input, a workflow can be designed providing access to formation enthalpies at different temperatures from the AFLOW-CCE tool [2].

[1] R. Friedrich et al., npj Comput. Mater. 5, 59 (2019).

[2] R. Friedrich et al., Phys. Rev. Mater. 5, 043803 (2021).

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