Effect of surface temperature on quantum dynamics of D2 on Cu(111) using a chemically accurate potential energy surface

The effect of surface mode vibrations on the reactive scattering of D-2, initialized in the ground rovibrational state (v = 0, j = 0), from a Cu(111) surface is investigated for different surface temperature situations. We adopt a time and temperature dependent effective Hamiltonian [Dutta et al., J. Chem. Phys. 154, 104103 (2021)] constructed by combining the linearly coupled many oscillator model [Sahoo et al., J. Chem. Phys. 136, 084306 (2012)] and the static corrugation model [M. Wijzenbroek and M. F. Somers, J. Chem. Phys. 137, 054703 (2012)] potential within the mean-field approach. Such an effective Hamiltonian is employed for six-dimensional quantum dynamical calculations to obtain temperature dependent reaction and state-to-state scattering probability profiles as a function of incidence energy of colliding D-2 molecules. As reported in the experimental studies, the movements of surface atoms modify the dissociative scattering dynamics at higher surface temperature by exhibiting vibrational quantum and surface atoms' recoil effects in the low and high collision energy domains, respectively. Finally, we compare our present theoretical results with the experimental and other theoretical outcomes, as well as discuss the novelty of our findings. Published under an exclusive license by AIP Publishing.

Automated summary

The effect of surface mode vibrations on the reactive scattering of D-2 from a Cu(111) surface is investigated for different surface temperature situations. The study reveals that the movements of surface atoms modify the dissociative scattering dynamics at higher surface temperature by exhibiting vibrational quantum and surface atoms' recoil effects.