Multimetallic Molecules, Reticular Materials,

and the Modern Modeling Frontier

Abstract: 

I will first describe advancements in electronic structure theory, focusing on the exploration of multimetallic molecular systems characterized by strong electron correlation. A specific case study will delve into the exploration of antiferromagnetic and ligand field effects on spin crossover in a dimeric Cr(II) complex [1] using multiconfigurational methods. In the second part I will describe the synergies of theory, computation, and machine intelligence to expedite the discovery of innovative metal-organic frameworks, with a particular focus on their application in catalysis [2] and water harvesting [3].

[1] A. Sarkar, M. R. Hermes, C. J. Cramer, J. S. Anderson, and L. Gagliardi Understanding Antiferromagnetic and Ligand Field Effects on Spin Crossover in a Triple-Decker Dimeric Cr(II) Complex J. Am. Chem. Soc. 2023, 145, 41, 22394–22402 DOI: 10.1021/jacs.3c05277

[2] K. E. McCullough, D. S. King, S. Chheda, M. S. Ferrandon, T. A. Goetjen, Z. H. Syed, T. R. Graham, N. M. Washton, O. K. Farha, L. Gagliardi, and M. Delferro High-throughput Experimentation, Theoretical Modeling, and Human Intuition: Lessons Learned in Metal-Organic Framework-Supported Catalyst Design, ACS Central Science 2023 9, 266–276 DOI: 10.1021/acscentsci.2c01422

[3] N. Hanikel, D. Kurandina, S. Chheda, Z. Zheng, Z. Rong, S. E. Neumann, J. Sauer, J. I. Siepmann, L. Gagliardi, and O. M. Yaghi, MOF Linker Extension Strategy for Enhanced Atmospheric Water Harvesting, ACS Central Science 2023, 9, 551–557, DOI: 10.1021/acscentsci.3c00018