Plasma-surface interactions in Cl- and Br-based plasmas have been studied for advanced front-end-of-line (FEOL) etching processes in nanoscale ULSI device fabrication. A Monte Carlo-based atomic-scale cellular model (ASCeM) was developed to simulate the feature profile evolution on nanometer scale during Si etching in Cl(2) and Cl(2)/O(2) plasmas, including surface oxidation, inhibitor deposition, and ion reflection and penetration on surfaces. A classical molecular dynamics (MD) simulation for Si/Br and Si/HBr as well as Si/Cl systems was also developed, along with an improved Stillinger-Weber interatomic potential model for Si/halogen interactions, to clarify surface reaction kinetics on atomic scale during Si etching in Cl(2) and HBr plasmas. The numerical results revealed the origin of profile or surface anomalies such as microtrench, roughness, and residue, and also etching fundamentals such as etch yield, product stoichiometry, and atomistic surface structures. Moreover, the etching of high-k dielectric and metal electrode materials, such as HfO(2) and TaN, was investigated in BCl(3)- and Cl(2)-containing plasmas with and without rf biasing, to gain an understanding of the etch mechanisms and to achieve anisotropic and selective etching of metal/high-k gate stacks. (C) 2009 Elsevier B.V. All rights reserved.