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Projet Labex PALM

Projet Labex PALM

Federica Agostini a obtenu un financement dans le cadre de l’appel à projet 2018 du Labex PALM.

The reaction of ground-state oxygen O(3P) with ethylene [1] encloses all the relevant and most challenging features of excited-state dynamical phenomena. Upon collision with energetic oxygen atoms, reaction paths involving electronic excited states are opened. Due to the ultrafast motion of the nuclei, transient products are short-lived, but important to determine in order to predict all possible channels for relaxation of the excited states to the ground state. For a full-dimensional excited-state simulation of the process, it is essential to capture the coupling among electronic states with different spin multiplicity, i.e., intersystem crossings, along with standard avoided crossings and conical intersections among singlet states (internal conversions). This project aims at developing a theoretical and computational tool allowing for quasiclassical simulations of the reaction of atomic oxygen in the triplet state with ethylene. The coupled-trajectory mixed quantum-classical (CT-MQC) algorithm, recently [2, 3] developed in the framework of the exact factorization of the electron-nuclear wavefunction [4], will be employed, as it has been shown to capture features of the coupled electron-nuclear motion involving electronic excited states that are usually missed by standard methods [5]. In parallel, the performance of time-dependent density functional theory as electronic structure method used to predict available electronic states and to capture intersystem crossings will be thoroughly investigated.

[1] B. Fu, Y.-C. Han, J. M. Bowman, L. Angelucci, N. Balucani, F. Leonori, and P. Casavecchia, Proc. Nat. Ac. Sci. 109, 9733 (2012).
[2] S. K. Min, F. Agostini, and E. K. U. Gross, Phys. Rev. Lett. 115, 073001 (2015).
[3] F. Agostini, S. K. Min, A. Abedi, and E. K. U. Gross, J. Chem. Theory Comput. 12, 2127 (2016).
[4] A. Abedi, F. Agostini, Y. Suzuki, and E. K. U. Gross, Phys. Rev. Lett. 110, 263001 (2013).
[5] S. K. Min, F. Agostini, I. Tavernelli, and E. K. U. Gross, J. Phys. Chem. Lett. 8, 3048 (2017).