ELUCIDATING MECHANISMS OF GAS-PHASE REACTIONS WITH DYNAMICS SIMULATIONS

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2024

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This thesis focuses on enhancing our understanding of chemical reaction dynamics through computational methods, addressing the limitations inherent in experimental techniques. While experimental methods provide valuable insights, they often lack the resolution and sensitivity required to capture the full complexity of chemical reactions.To predict and analyze reaction dynamics more effectively, computational studies initially employ Potential Energy Surface (PES) calculations. PES is instrumental in mapping the energy landscapes that govern chemical reactions, helping to visualize how potential energy varies with molecular configurations and to identify stable intermediates, transition states, and energy barriers. However, PES calculations have limitations, especially in dynamically complex systems where assumptions such as a maintained statistical ensemble for all intermediates do not hold. Situations involving non-Intrinsic Reaction Coordinate behaviors, insufficient intramolecular vibrational redistribution, and direct reactions without long-lifetime intermediate formations where PES alone may not provide complete insights. In response to these challenges, Ab Initio Molecular Dynamics (AIMD) simulations are employed. AIMD goes beyond the limitations of PES by simulating a statistical ensemble of trajectories that reflect experimental conditions, including various impact parameters and orientations of collisions. This method calculates the interactions between atoms using ab initio techniques and updates atomic positions iteratively based on classical equation of motion. By allowing the real-time tracking of atomic motions, AIMD provides a dynamic and detailed view of the molecular transformations during reactions which are often challenging to model with PES-based methods.

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Chemistry, Computational chemistry, Physical chemistry

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326 pages

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