Molecular self-assembly in aqueous systems arises from a delicate interplay of entropic and enthalpic effects associated with the structuring of water. This interplay also underlies many of the remarkable macroscopic material responses to molecular cues that are encountered in biological systems. Recently, new insight into self-assembly of amphiphilic molecules in an alternative class of structured solvents, specifically nematic solvents, has been reported. The presence of long-range orientational order in nematic solvents was shown to open new avenues to control of molecular assemblies that are not possible in aqueous systems. One key opportunity revolves around the formation of topological defects in nematic solvents, which can serve as virtual templates for triggering and hosting molecular assemblies. Motivated by these observations, this proposal seeks to develop a fundamental understanding of equilibrium and dynamic aspects of molecular self-assembly of amphiphiles in defects of nematic solvents, and to leverage that understanding to demonstrate principles that permit formation of single nanoscopic assemblies to be amplified into macroscopic outputs. The approach described in this proposal builds from recent observations by PI Abbott that the nanoscopic cores of topological defects formed in nematic solvents, which are molecularly disordered relative to bulk nematic solvents, selectively trigger cooperative self-assembly of amphiphiles. These observations generate a range of questions regarding the equilibrium and dynamic properties of these assemblies, the answers to which will enable development of new principles for amplification of signals across multiple time and length scales. The research is organized into three parts.