Layered hybrid metal-organic chalcogenolates (MOChas) present a versatile platform for exploring and engineering exceptional light-matter interactions, offering opportunities to design materials for advanced photonic and quantum technologies. This presentation will highlight our synthetic efforts to expand the library of MOChas, focusing on the development of 50 structurally diverse systems. By leveraging cutting-edge serial femtosecond crystallography (smSFX), we have elucidated the intricate relationships between ligand chemistry, structural distortions, and their resulting optical properties. These insights are critical for identifying design rules that govern excitonic and polaritonic behavior in MOChas, with an emphasis on tuning their photophysical properties for targeted applications. We will reveal how smSFX has enabled directed self-assembly of new materials opening the door to more precise control over their excitonic parameters, including energy, lifetime, and coupling strength. The data obtained from smSFX has provided an unprecedented understanding of how ligand-induced distortions affect lightmatter interactions, forming the basis for predictive materials design. This work underscores the power of co-design strategies that integrate synthetic chemistry, structural analysis, and computational modeling to accelerate the development of next-generation materials. This talk will showcase the synergistic integration of experimental and computational approaches in MOCha research, providing a pathway to the rational design of materials with exceptional nonlinear optical properties and quantum functionality. Finally, the potential for ultrafast electronic dynamics using the unique capabilities of X-ray free electron laser (XFEL) small molecule crystallography will be considered.
J. Nathan Hohman earned his PhD in chemistry from the Pennsylvania State University in 2011, specializing in the synthesis, structure, and dynamics of ultrathin self-assembled monolayers. After a postdoctoral appointment at Stanford University department of Materials Science and Engineering investigating nanostructures for brain-machine interfaces, he joined the Molecular Foundry at Berkeley Laboratory in 2015, and led a group specializing in the systematic control and design of dimensionality and connectivity of metal-organic chalcogenolate assemblies (MOCha), inorganic coordination polymers that pair the crystallinity and ease of growth of inorganic materials with the systematic intervention into the structure/function relationships intrinsic to soft matter. Now at the University of Connecticut Department of Chemistry, his group aims to leverage the properties of hybrid materials to address the challenges in understanding energy, mass, and information transport in extended material systems.