Hyojun Choi, Ju Yong Park, Jaewook Lee, Hyun Woo Jeong, Kun Yang, Sun Young Lee, Dong Han, Heejin Hong, Young Yong Kim, Min Hyuk Park
Ferroelectricity in (Hf,Zr)O2 thin films is highly sensitive to bottom-electrode chemistry, as interfacial redox reactions during atomic layer deposition (ALD) and subsequent annealing can generate defective interlayers and alter oxygen-vacancy distributions. Here, we propose a stoichiometry- and lattice-tunable molybdenum nitride (MoNx) electrode platform that enables single-layer interfacial engineering through control of the Mo:N ratio. MoNx films with x = 0.00, 0.05, 0.52, and 0.79 (denoted as Mo, 05MoN, 52MoN, and 79MoN) were sputter-deposited and integrated into symmetric MoNx/Hf0.5Zr0.5O2/MoNx capacitors containing 8 nm-thick ALD Hf0.5Zr0.5O2. Structural analysis confirms a transition from Mo (110)-textured films to rock-salt-type MoNx with a (111) texture at higher N contents, while electrode-grade resistivity is maintained (≤ 200 μΩ∙cm for 52MoN). Chemical analyses reveal that increasing the N content substantially suppresses ALD-induced electrode oxidation and reduce the thickness of the oxidized interfacial-layer by 47.7% for 52MoN relative to Mo; N incorporation into the Hf0.5Zr0.5O2 (HZO) near the bottom interface is also detected. Consistently, the monoclinic phase fraction decreases from ~ 21% for Mo to < 5% for 52MoN and 79MoN. All capacitors exhibit minimal wake-up, with a ≤ 3.0% change in double remanent polarization after 104 cycles at 3 MV∙cm-1. Benchmarking against other stoichiometry-controlled electrode systems (e.g., TaNx, RuOx, and TiNx) shows that the MoNx platform maintains high pristine polarization (> 47.5 μC∙cm-2) while suppressing wake-up across a wide compositional range. Endurance improves markedly with N content, reaching ~ 108-109 cycles for high-N MoNx electrodes, depending on the cycling voltage. These results establish MoNx as a scalable, composition-engineerable electrode system that couples interfacial microstructure control with enhanced ferroelectric reliability in HZO thin films.