Multi-scale modeling of early-stage morphology in solution-processed polycrystalline thin films

Area of Science:

• Materials Science
• Chemical Engineering
• Physics

Background:

• Submonolayer polycrystalline films are crucial in various applications.
• Understanding nucleation and growth kinetics is key for controlling film properties.
• Solution-phase processing offers versatile fabrication methods.

Purpose of the Study:

• To develop a predictive model for early-stage nucleation, growth kinetics, and mesoscale domain structure in solution-processed submonolayer polycrystalline films.
• To combine stochastic nucleation with deterministic diffusion dynamics.
• To validate the model against experimental data.

Main Methods:

• A hybrid model integrating classical nucleation theory with a 2D diffusion equation.
• Numerical solution of the diffusion equation, treating nuclei as monomer sinks.
• Comparison with experimental measurements of solution-processed submonolayer tetracene films using vapor-liquid-solid deposition.

Main Results:

• Excellent agreement between model predictions and experimental observations.
• Accurate prediction of distinct induction, nucleation, and growth regimes.
• Precise matching of nucleation onset time, domain density, and domain spacing statistics.
• Detailed insights into the evolving monomer concentration landscape and derived rates.

Conclusions:

• The developed model provides a robust framework for understanding and predicting film formation in solution-processed submonolayer polycrystalline films.
• The model successfully captures key kinetic and structural characteristics, validating its predictive power.
• This work offers a valuable tool for optimizing fabrication processes and material design.