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Thrust 4: Predictive Science of Synthesis

Project work in this thrust will focus on theoretical framework and simulation tools that maintain the fidelity of molecular simulations to predict ensemble and macromolecular behavior during nucleation, phase separation, and self-assembly—a bottom-up approach to materials synthesis.

Projects

Predictive Understanding of Self-assembly: Particle-mediated Growth

KM Rosso, D Li, ML Sushko, J Chun, Z. Shen, Z Wang

We aim to develop a fundamental understanding of particle-based growth of crystalline materials from aqueous solution, ultimately to learn how to control the assembly of new materials. The project focuses on measuring and modeling inter-particle forces in situ, and understanding how those forces lead to orientation-selective attraction and adhesion. Scanned probe measurements of force combined with multiscale simulations will yield insights that enable formulation of new material design principles. This includes directed synthesis of mesoscale architectures with nanoscale functioning units, which could spur new advances in energy technologies (e.g., electrochemical storage, solar energy capture). Because of simultaneous relevance to mineral growth in geosciences, understanding the particle-based growth pathway will also enable a transformation in understanding growth/dissolution processes with impacts ranging from soil evolution and mineral phase stabilities and reactivity, to rheological properties of rocks and minerals.

Thrust 4: Predictive Science of Synthesis, Image 1
A sequence of high resolution liquid cell transmission electron microscopy (HRTEM) images of the intrinsically nanophase mineral ferrihydrite in aqueous solution undergoing oriented aggregation starting from the attractively captured solvent-separated state (a), to improved interparticle alignment (b), to initial adhesion under near perfect alignment (c), to interface restructuring (d), and finally to perfectly aligned and fused crystallites (e). From  Li D, MH Nielsen, JRI Lee, C Frandsen, JF Banfield, and  JJ De Yoreo. 2012. "Direction-Specific Interactions Control Crystal Growth by Oriented Attachment" Science, 336, 1014-1018. DOI: 10.1126/science.1219643.  Reprinted with permission from AAAS*.

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Fundamental Mechanisms of Nucleation and Growth of Particles in Solution

MD Baer, AJ Karkamkar, CJ Mundy, SM Kathmann, GK Schenter, and JJ DeYoreo

We will focus on the use of molecular models to mimic and better understand the underlying molecular-to-mesoscale principles of assembly of open-framework inorganic oxide supports and their related surface-grafted organometallic fragments. Such molecular models will provide new insight into the whole pathway and energetic controls on nucleation in solution media. This understanding of equilibrium and nonequilibrium synthesis of materials in aqueous electrolytes will significantly enhance our ability to control processes that lead to self-assembly and scalable synthesis of new catalytic materials with novel properties.

Coupling of multiple scales that gives rise to particle formation. Intrinsic ion solvation (lower left) influences ion-surface interactions (top left) modifying collective interactions that lead to formation of nanoassemblies (right schematic and photo). Photo courtesy of Jun Liu.
Coupling of multiple scales that gives rise to particle formation. Intrinsic ion solvation (lower left) influences ion-surface interactions (top left) modifying collective interactions that lead to formation of nanoassemblies (right schematic and photo). Photo courtesy of Jun Liu.

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