Hierarchical Multicomponent Inorganic Metamaterials: Intrinsically Driven Self-Assembly at the Nanoscale

Increasingly intricate in their composition and structural organization, hierarchical multicomponent metamaterials with nonlinear spatially reconfigurable functionalities challenge the intrinsic constraints of natural materials, revealing tremendous potential for the advancement of biochemistry, nanophotonics, and medicine. Recent breakthroughs in high-resolution nanofabrication utilizing ultranarrow, precisely controlled ion or laser beams have enabled assembly of architectures of unprecedented structural and functional complexity, yet costly, time- and energy-consuming high-resolution sequential techniques do not operate effectively at industry-required scale. Inspired by the fictional Baron Munchausen's fruitless attempt to pull himself up, it is demonstrated that metamaterials can undergo intrinsically driven self-assembly, metaphorically pulling themselves up into existence. These internal drivers hold a key to unlocking the potential of metamaterials and mapping a new direction for the large-area, cost-efficient self-organized fabrication of practical devices. A systematic exploration of these efforts is presently missing, and the driving forces governing the intrinsically driven self-assembly are yet to be fully understood. Here, recent progress in the self-organized formation and self-propelled growth of complex hierarchical multicomponent metamaterials is reviewed, with emphasis on key principles, salient features, and potential limitations of this family of approaches. Special stress is placed on self-assembly driven by plasma, current in liquid, ultrasonic, and similar highly energetic effects, which enable self-directed formation of metamaterials with unique properties and structures.