0000000000254351
AUTHOR
Erwan Privat
Dependence on collision energy of the stereodynamical properties of the 18O + 32O2 exchange reaction
We report a quantum stereodynamical study of the 18O + 16O16O(v = 0, j = 1) → 18O16O(v′ = 0, j′) + 16O oxygen exchange reaction at four different collision energies. We calculated the polarisation ...
Quantum dynamics of the oxygen isotopic exchange : lifetimes of metastable states of the ozone intermediate complex
This thesis aims to describe the ozone dynamics during the isotopic exchange reactions of oxygen of type xO + yO zO (xO yO zO)* xO yO + zO, where x, y and z are the atomic masses of the stable oxygen isotopes (16, 17, 18). Firstly, we analyze several methods of accurate description of the atom interactions and numerical schemes to obtain the observables for the collision. Then, in a full-quantum hyperspherical formalism, we study the actual dynamics of the reactive process O + O2 -> O3* -> O2 + O. The metastable ozone created can then either decompose into oxygen by the inverse reaction, or relax into stable ozone by exchanging energy with the environment, typically N2 or O2 molecules. Thes…
Direct time delay computation applied to the O + O2 exchange reaction at low energy: Lifetime spectrum of O3* species
We report full quantum dynamical calculations for lifetimes of scattering resonances, among which are true metastable states, of the intermediate heavy ozone complex 50O3* of the 18O + 16O16O reaction, for any value of the total angular momentum quantum number J. We show that computations for nonzero values of J are mandatory in order to properly analyze resonances and time delays, with a view to establish a somewhat comprehensive eigenlife spectrum of the complex O3*. Calculations have been performed in a given low to moderate energy range, including the interval between zero-point energies (ZPEs) of reagents and product species. Quasi-bound states tend to be more numerous, and eigenlifeti…
Quantum stereodynamics of the 18O+16O16O→16O18O+16O exchange reaction at low collision energy
Abstract We present a quantum study of stereodynamics of the 18 O + 16 O 16 O ( v = 0 , j = 1 ) → 16 O 18 O ( v ′ = 0 , j ′ ) + 16 O exchange reaction at a collision energy E coll = 0.01 eV . Polarization moments of the reactants have been computed and stereodynamical portraits have been generated. The results show that the reactant preferred relative orientations are strongly dependent on the scattering angle and on the product rotational states.
Extension of the Launay Quantum Reactive Scattering Code and Direct Computation of Time Delays.
Scattering computations, particularly within the realm of molecular physics, have seen an increase in study since the development of powerful quantum methods. These dynamical processes can be analyzed via (among other quantities) the duration of the collision process and the lifetime of the intermediate complex. We use the Smith matrix Q = -iℏS†dS/dE calculated from the scattering matrix S and its derivative with respect to the total energy. Its real part contains the state-to-state time delays, and its eigenvalues give the lifetimes of the metastable states [ Smith Phys. Rev. 1960 , 118 , 349 - 356 ]. We propose an extension of the Launay HYP3D code [ Launay and Le Dourneuf Chem. Phys. Let…