Computational Workflows for an Accelerated Design of Novel Materials and Interfaces

The development of automated computational tools is required to accelerate the discovery of new functional materials, to speed up the transition to a sustainable future. Here, I address this topic by designing new electrodes with controlled interfaces for different applications which accelerate the transition to a sustainable future. These workflows are implemented in the framework of Density Functional Theory (DFT), using MyQueue and the Atomistic Simulation Environment (ASE). In the first part of my talk, starting from our recent work on a fully autonomous workflow, which identifies materials to be used as intercalation electrodes in batteries, based on thermodynamic and kinetic descriptors like adsorption energies and diffusion barriers,¹ I will describe a new modular approach to estimate electronic and ionic mobility in energy materials useful for a variety of applications, from batteries and fuel cells and solar energy conversion and storage. A substantial acceleration for the calculations of the kinetic properties has been obtained due to a recent implementation of the Nudged Elastic Bands (NEB) method, which takes into consideration the symmetries of the system to reduce the number of images to calculate. Moreover, we have established a surrogate model to identify the transition states, which can further reduce the computational cost to at least one order of magnitude.^2,3 In the second part of my talk, I discuss how engineering the interface can positively impact surface properties for electrochemical water splitting: I apply strain engineering and external stimuli to switch material’s polarization to decrease the reaction overpotential in oxynitride materials for the oxygen evolution reaction.^5,6 In the last part of my talk, I will describe my vision for autonomous computational workflows, namely the creation of workflows for interface and their integration with experimental workflows.<br/> <br/><b>References</b><br/>[1] F. T. Bölle, N. R. Mathiesen, A. J. Nielsen, T. Vegge, J. M. García-Lastra, and I. E. Castelli, Batteries & Supercaps 3, 488 (2020).<br/>[2] F. T. Bölle, A. Bhowmik, T. Vegge, J. M. García-Lastra, and I. E. Castelli, Batteries & Supercaps 4, 1516 (2021).<br/>[3] B. H. Sjølin, P. B. Jørgensen, A. Fedrigucci, T. Vegge, A. Bhowmik, and I. E. Castelli, Batteries &Supercaps 2023, e202300041 (2023).<br/>[4] Z. Lan, D. R. Småbråten, C. Xiao, T. Vegge, U. Aschauer, and I. E. Castelli, ACS Catal 11, 12692<br/>(2021).<br/>[5] C. Spezzati, Z. Lan, and I. E. Castelli, Journal of Catalysis 413, 720 (2022).