Theme 1 colloquium: Molecular Dynamics Simulations for Uni- and Bi-Molecular Reactivity

Tuesday 2 July 2024, 4 pm

In this colloquium, I will present recent theoretical advances in studying the fundamental processes related to chemical reactivity. In particular, I will focus on two fundamental processes: unimolecular fragmentation and ion-molecule reactive processes. 

A first example, is the possibility of forming protonated glycine from ion-molecule reactions. We combined direct dynamics of bi- and uni-molecular fragmentation with IRMPD experiments to shed some light on the possibility of forming glycine (and some isomers) via the simple reaction between protonated hydroxilamine and acetic acid. 

Then I will show how reaction barriers can be accurately obtained from simulations but one needs to include some nuclear quantum effects.

Finally, I will give some examples on how rate constants and free energy profiles can be modified when nuclear quantum effects are included at both room and low temperatures.

References

  1. Y.Jeanvoine, A.Largo, W.L.Hase and R.Spezia. J. Phys. Chem. A 122, 869-877 (2018). 
  2. D.Scuderi, A.F.Perez-Mellor, J.Lemaire, S.Indrajith, J.-X.Bardaud, A.Largo, Y.Jeanvoine and R.Spezia. ChemPhysChem21, 503-509 (2020).
  3. A.Malik, R.Spezia and W.L.Hase. J. Am. Soc. Mass Spectrom. 32, 169-179 (2021). 
  4. F.Angiolari, S.Huppert and R.Spezia. Phys. Chem. Chem. Phys. 24, 29357-29370 (2022). 
  5. F.Angiolari, S.Huppert, F.Pietrucci and R.Spezia. J. Phys. Chem. Lett. 14, 5102–5108 (2023). 
  6. F.Angiolari, G.Mandelli, S.Huppert, C.Aieta and R.Spezia. Submitted. Preprint on ChemRXiv: https://10.26434/chemrxiv2024-wb68d