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Abstract: Collective behavior in large ensembles of network-coupled dynamical systems remains an active area of research in the nonlinear dynamics and networks science communities. Example applications include both naturally-occurring and man-made systems, e.g., cardiac pacemakers, synthetic cell engineering, and power grids. Researchers’ efforts have illuminated rich nonlinear phenomena in heterogeneous oscillator systems, but important practical questions remain, including: (i) How can heterogeneous oscillator networks be optimized for synchronization? and (ii) What is the most efficient protocol for controlling heterogeneous oscillator networks? In this talk I will explore these important questions and highlight a number of surprising outcomes. Central to this work is the development of the Synchrony Alignment Function, a theoretical tool and objective measure of collective behavior that quantifies the interplay between a complex network structure and the heterogeneous internal dynamics of each oscillator. We’ll explore grass-roots methods for optimizing synchronization dynamics, applicability to limit-cycle and chaotic oscillators, and dual approaches to network control.