Microscopic Modeling, Machine Learning-Based Modeling and Optimal Operation of Thermal and Plasma Atomic Layer Deposition

Atomic layer deposition (ALD) and plasma enhanced atomic layer deposition (PEALD) are the most widely utilized deposition techniques in the semiconductor industry due to their superior ability to produce highly conformal films and to deposit materials into high aspect-ratio geometric structures. Additionally, plasma enhanced ALD is able to further speed up the deposition process and to reduce the temperature requirement through the utilization of high energy particles. However, ALD and PEALD experiments remain expensive and time-consuming, and the existing first-principles based models have not yet been able to provide solutions to key process outputs that are computationally efficient, which is necessary for on-line optimization and real-time control. Motivated by the above considerations, this dissertation focuses on addressing these issues for both ALD and PEALD. First, for ALD, the development of key components of a comprehensive simulation framework is presented. The simulation framework integrates first-principles-based microscopic modeling, input/output modeling and optimal operation of thermal atomic layer deposition (ALD) of SiO2 thin-films using bis(tertiary-butylamino)silane (BTBAS) and ozone as precursors. Specifically, we initially utilize Density Functional Theory (DFT)-based calculations for the computation of the key thermodynamic and kinetic parameters, which are then used in the microscopic modeling of the ALD process. Subsequently, a detailed microscopic model is constructed, accounting for the microscopic lattice structure and atomic interactions, as well as multiple microscopic film growth processes including physisorption, abstraction and competing chemical reaction pathways. Kinetic Monte-Carlo (kMC) algorithms are utilized to obtain computationally efficient microscopic model solutions while preserving model fidelity. The obtained kMC simulation results are used to train Artificial Neural Network (ANN)-based data-driven models that capture the relationship between operating process parameters and time to ALD cycle completion. Specifically, a two-hidden-layer feed-forward ANN is constructed to find a feasible range of ALD operating conditions accounting for industrial considerations, and a Bayesian Regularized ANN is constructed to implement the cycle-to-cycle optimization of ALD cycle time. Extensive simulation results demonstrate the effectiveness of the proposed approaches. The kMC models successfully achieves a growth per cycle (GPC) of 1.8 A per cycle, which is in the range of reported experimental values. The ANN models accurately predict deposition time to steady-state from the given operating condition input, and the cycle time optimization using BRANN model reduces the conventional BTBAS cycle time by 60%. After developing an efficient simulation framework, a more detailed study on the optimal operation policy is performed using a multiscale data-driven model. The multiscale data-driven model captures the macroscopic process domain dynamics with a linear parameter varying model, and characterizes the microscopic domain film growth dynamics with a feed-forward artificial neural network (ANN) model. The multiscale data-driven model predicts the transient deposition rate from the following four key process operating parameters that can be manipulated, measured or estimated by process engineers: precursor feed flow rate, operating pressure, surface heating, and transient film coverage. Our results demonstrate that the multiscale data-driven model can efficiently characterize the transient input-output relationship for the SiO2 thermal ALD process using Bis(tertiary-butylamino)silane (BTBAS) as the Si precursor. The multiscale data-driven model successfully reduces the computational time from 0.6 - 1.2 hr for each time step, which is required for the first-principles based multiscale computational fluid dynamics (CFD) model, to less than 0.1 s, making its real-time usage feasible. The developed data-driven modeling methodology can be further generalized and used for other thermal ALD or similar deposition systems, which will greatly enhance the feasibility of industrial manufacturing processes.For PEALD, a similar methodology is adopted. First, an accurate, yet efficient kinetic Monte Carlo (kMC) model and an associated machine learning (ML) analysis are proposed to capture the surface deposition mechanism of the HfO2 thin-film PEALD using Tetrakis-dimethylamino-Hafnium (TDMAHf) and oxygen plasma. Density Functional Theory (DFT) calculations are performed to obtain the key kinetic parameters and the structural details. After the model is validated by experimental data, a database is generated to explore a variety of precursor partial pressure and substrate temperature combinations using the kMC algorithm. A feed-forward Bayesian regularized artificial neural network (BRANN) is then constructed to characterize the input-output relationship and to investigate the optimal operating condition. Next, based on an associated work on a comprehensive 3D multiscale computational fluid dynamics (CFD) model for the PEALD process, a 2D axisymmetric reduction of the previous 3D model of PEALD reactors with and without the showerhead design has been adopted to enhance the computational efficiency. Using the derived 2D CFD model, a data-driven model is constructed based on a recurrent neural network (RNN) for process characterization. The developed integrated data-driven model is demonstrated to accurately characterize the key aspects of the deposition process as well as the gas-phase transport profile while maintaining computational efficiency. The derived data-driven model is further validated with the results from a full 3D multiscale CFD model to evaluate model discrepancy. Using the data-driven model, an operational strategy database is generated, from which the optimal operating conditions can be determined for the deposition of HfO2 thin-film based on an elementary cost analysis