Modeling Phase Transformation in Complex Oxides with Charge-Informed Interatomic Potential

When and Where

Nov 28, 2023
10:45am - 11:00am

Sheraton, Second Floor, Back Bay A



Peichen Zhong1,Bowen Deng1,Gerbrand Ceder1

University of California Berkeley1


Peichen Zhong1,Bowen Deng1,Gerbrand Ceder1

University of California Berkeley1
Disordered rocksalt materials represent the most promising earth-abundant cathode materials for Li-ion batteries, potentially enabling the scaling of Li-ion energy storage to numerous TWh/year production. These advanced battery materials often comprise multiple elements and exhibit significant site disorder and structure complexity. Mn-rich DRX cathodes have observed a phase transformation from disorder to partial spinel-like order during charge/discharge cycling. To understand this phenomenon and reveal the underlying physics, we employed atomistic modeling with charge information derived from ab-initio calculations.<br/><br/>CHGNet is a novel machine-learning interatomic potential (MLIP) with atomic charge inference from magnetic moments. The explicit incorporation of magnetic moments allows CHGNet to learn and accurately represent the orbital occupancy of electrons, thereby enhancing its ability to describe both atomic and electronic degrees of freedom. We fine-tuned the pre-trained universal CHGNet within the Li-Mn-Ti-O-F chemical space using high-fidelity DFT calculations. The fine-tuned CHGNet was then applied to Li<sub>1.1-x</sub>Mn<sub>0.8</sub>Ti<sub>0.1</sub>O<sub>1.9</sub>F<sub>0.1</sub> DRX system, using charge-informed molecular dynamics to investigate the structural ordering change, charge distribution, and electrochemical properties of the transformed DRX compounds.

Symposium Organizers

Mathieu Bauchy, University of California, Los Angeles
Ekin Dogus Cubuk, Google
Grace Gu, University of California, Berkeley
N M Anoop Krishnan, Indian Institute of Technology Delhi

Symposium Support

Patterns and Matter | Cell Press

Publishing Alliance

MRS publishes with Springer Nature


Symposium Support