CAREER: Angstrom-Precise Manufacturing Guided by Incommensurate Interfaces and Surfaces in Two-dimensional Layered Materials

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This Faculty Early Career Development (CAREER) grant supports the investigation of scalable additive and subtractive manufacturing processes with extreme (sub-nanometer, Ångström-scale) precision in two-dimensional layered materials. Novel materials processing methods stemming from this research will broadly benefit U.S. advanced manufacturing through newfound ability to deterministically and scalably manipulate matter at unprecedented length scales, thereby greatly impacting high-technology sectors such as biopharmaceuticals, optoelectronics, and semiconductor manufacturing. The resulting new knowledge from this fundamental research advances capabilities to manufacture materials with Ångström-precise features, such as highly-uniform nano-pore, nano-channel, and nano-island arrays, achieving ultimate resolution and scales not currently attainable through state-of-the-art techniques. The integration of research with educational and outreach initiatives, including the development of children’s read-along books and research engagement with underrepresented/underprivileged middle-school, community college and veteran students, collectively help foster the training of a diverse and globally-competitive advanced manufacturing workforce. The ever-growing diversity of two-dimensional layered materials (2DLMs) endows their versatility as the ultimate Ångström-scale building blocks for bottom-up, layer-by-layer additive and subtractive manufacturing with atomic precision and nearly limitless configurations. Uniquely, the atomically-thin, anisotropic nature of 2DLMs enables arbitrary engineering of Moiré domains via incommensurate interfaces, which opens novel routes for Ångström-precise feature patterning with deterministic control over the exact lattice geometry, atomic/molecular terminations, and local stoichiometries. Generalizable to arbitrary 2DLMs beyond the prototypical graphene, hexagonal boron nitride, transition-metal compounds, and numerous (M)Xenes, this research investigates the fundamental process-structure-property relations of highly-periodic, Ångström-precise features engineered via deterministic rotational/translational turbostratic misalignment. Empirical studies elucidate the mechanisms underlying the self-limiting and spatially-selective chemical functionalization (additive) and etching (subtractive) reactions with energetic plasma species that yield massively-parallel features, such as large-scale arrays of highly monodispersed nano-pores, nano-channels (subtractive), and nano-islands (additive). Scalability of this methodology is investigated through translating phenomena observed from nano/micron-scale samples to the processing of centimeter-scale 2DLM sheets, with the desired Ångström-precise morphologies informed through inverse design guided by machine learning models trained on process parameters and metrology data. The resulting capabilities to manipulate and manufacture Ångström-precise features in 2DLMs provide new pathways toward tailored molecular sieves and ultra-high-density devices and instrumentation platforms.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.