Lattice Matching Dictates the Growth Mode and Quality of Deuterium Crystallization in Confined Spherical Shells

Abstract

Cryogenic hydrogen isotope fuel layers with high structural integrity and atomic-scale smoothness are prerequisites for symmetric implosion and ignition in inertial confinement fusion (ICF). Using deuterium (D$_2$) as model fuel, we perform large-scale molecular dynamics simulations with a Feynman-Hibbs corrected Silvera-Goldman potential to describe nuclear quantum effects at low temperatures, systematically investigating D$_2$ crystallization inside spherical ablator capsules. By varying substrate lattice constant from 3.1 angstrom to 3.9 angstrom, we demonstrate that lattice matching dictates the transition from coherent epitaxial growth to polycrystalline formation, establishing it as the primary design principle for high-performance targets. When the substrate lattice closely matches the equilibrium hexagonal-close-packed (HCP) spacing of cryogenic D$_2$ (approximately 3.5 angstrom), D$_2$ forms coherent layer-by-layer epitaxial growth consistent with Ostwald's stepwise nucleation theory, yielding HCP-dominated near-single crystals with minimal dislocations and ultra-smooth inner surfaces. In contrast, large lattice mismatch destabilizes coherent growth and causes island-like growth, producing polycrystalline structures with mixed HCP/FCC phases, elevated defects, and greatly increased surface roughness. Radial stress analysis shows that interfacial stress from mismatch localizes within 2-3 molecular layers near the interface, triggering subsequent defect-mediated growth. These findings highlight substrate lattice matching in regulating confined solid growth and crystallization quality, establish it as a key principle for ablator inner-surface engineering in ICF cryogenic targets, and offer atomic guidance for growing high-quality single-crystal deuterium-tritium (DT) fuel layers with optimal smoothness.