The overarching goal of the Functional Polymer and Hybrid Architectures (FPHA) theme is to understand, design, and manipulate the multiscale self-assembly of macromolecular and hybrid materials to tailor electronic transport and response. The emphasis is on probing the mechanisms of self-assembly that are essential for the development of functional hybrid architectures of relevance to energy technologies, such as organic photovoltaics. The approach relies upon precision synthesis and characterization of organic building blocks and well-defined 2D material interfaces that are designed to reveal the atomistic and long-range interactions that govern assembly, the development of in situ optical spectroscopy and neutron scattering characterization methods to probe structure and properties, and the strong integration of computational theory and simulation to describe and guide experiments.

The FPHA theme is organized around three specific aims (1) To understand the role of non-covalent interactions in the self-assembly of energy-responsive macromolecular systems.  Here the focus is on substrate-free (solution-phase) assembly of conjugated molecular and polymeric systems, using expertise in synthetic chemistry within the Theme to tailor building blocks with rationally designed functional groups.  In situ characterization during self-assembly using neutron scattering will be employed to elucidate their structures and dynamics during the self-assembly process.  (2) To understand the role of hybrid interfacial interactions between organic components and substrates in directing self-assembly, and the impact on optoelectronic processes relevant to organic electronics.  Here, well-defined two-dimensional (2D) interfaces synthesized and characterized within the Theme will be introduced as well-defined interfaces to investigate how this alters the assembly of the tailored building blocks, to provide a direct comparison to self-assembly in solution.  In situ characterization techniques to understand the assembly processes are developed in both cases with a focus on optimizing charge transport in the assembled architectures. (3) To understand how chemical and physical information encoded at the nanoscale translates into soft matter structure, dynamics and function at meso- and macro-scales with predictive theory and simulation. Here new theoretical and computational capabilities are applied to develop multiscale theoretical and computational strategies that target the fundamental understanding (and ultimately the successful manipulation) of self-assembly of soft matter systems and hybrid materials. The dynamical evolution of structure and optoelectronic properties predicted from first principles will be coupled closely with what is learned from the tailored experimental synthesis and assembly – and the spatiotemporal feedbackprovided by in situ optical and neutron scattering characterization techniques – to accelerate the process of materials design

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