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This study explores hydrocarbon decomposition on iridium surfaces, crucial for graphene growth. Kinetic Monte Carlo and rate equation simulations, validated by experiments, reveal decomposition mechanisms and limitations for continuous growth methods.

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Area of Science:

  • Surface Science
  • Materials Science
  • Computational Chemistry

Background:

  • Hydrocarbon decomposition on Ir(111) is key for epitaxial graphene growth.
  • Understanding carbon feedstock behavior is vital for controlling graphene formation.

Purpose of the Study:

  • To determine the kinetics of hydrocarbon thermal decomposition on Ir(111).
  • To compare kinetic Monte Carlo (kMC) and rate equation simulation methods.
  • To validate theoretical models against experimental data and apply them to continuous dosing relevant for chemical vapor deposition (CVD).

Main Methods:

  • Density Functional Theory (DFT) calculations for energy barriers.
  • Kinetic Monte Carlo (kMC) simulations.
  • Rate equations modeling.
  • In situ X-ray Photoelectron Spectroscopy (XPS) for experimental validation.

Main Results:

  • Both kMC and rate equation models provide reasonable predictions for ethylene decomposition kinetics.
  • Rate equations show reduced reliability at higher hydrocarbon coverages.
  • Adjusting DFT-derived energy barriers improves agreement between theoretical and experimental results.
  • Continuous dosing simulations predict C monomer formation, limited by hydrogen presence for ethylene and methane.

Conclusions:

  • kMC simulations offer a more robust approach for complex surface reactions, especially at higher coverages.
  • DFT energy barrier adjustments are necessary for accurate theoretical predictions.
  • The study elucidates mechanisms for graphene growth precursors, applicable to CVD processes.