Ting-Yun WangChun-Ho ChuangChi-Lin MoYu-Sen JiangJing-Jong ShyueTZONG-LIN JAY SHIEHMIIN-JANG CHEN2025-01-032025-01-032025-01https://www.scopus.com/record/display.uri?eid=2-s2.0-85211572343&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/724528Zr-doped HfO2-based ferroelectric materials demonstrate substantial potential for next-generation nonvolatile memory applications. However, the layer-by-layer doping method used in conventional atomic layer deposition (ALD) is restricted by the finite number of available deposition cycles for doping, which obstructs the progress of ultrathin films necessary for scaling down devices. In this paper, we propose a novel alternating multi-pulse (AMP) ALD approach that incorporates Zr doping into each ALD cycle, resulting in a homogeneous dopant distribution throughout the film thickness and improved areal coverage of precursors. By alternating the pulsing sequence of Hf and Zr precursors in each ALD cycle, significant ferroelectricity is achieved in the thin film with a high Zr/Hf ratio. Furthermore, a multi-pulse doping model is developed to elucidate the doping mechanism in AMP ALD, which is supported by the atomic percentages obtained from X-ray photoelectron spectroscopy and the measured growth rate per cycle. The AMP ALD technique provides an innovative solution for achieving continuous and tunable doping, rather than discrete or digital doping, which is critical for ultra-scale materials and devices.falseAlternating multi-pulse dopingAtomic layer depositionFerroelectricityNanoscale thin filmsZr-doped HfO2[SDGs]SDG7journal article10.1016/j.mtchem.2024.1024592-s2.0-85211572343