Vibrationally enhanced associative photodesorption of molecular hydrogen from Ru(0001)

摘要: Abstract The effect of vibrational excitation, for example by infrared (IR) laser pulses, on the photodesorption H2 and D2 from a Ru(0 0 0 1) surface has been investigated theoretically. Based information first principle electronic structure theory, minimal two-mode two-state model is developed Desorption Induced Electronic Transitions (DIET) in single-excitation limit. In model, finite excited state lifetime few femtoseconds (fs) accounted averaging scheme. Using ground as initial averaging, energy partitioning into different degrees freedom isotope effects are investigated. We then consider vibrationally states wavepackets states, which found to have large influence outcome reaction. To show that IR excitation adsorbates feasible, we use optimal control theory design pulses sub-picosecond range. For these, relaxation due coupling adsorbate vibrations electron–hole pairs metal for. Our major result isotope- bond-selective photoreactions should be possible some extent, even strongly dissipative media.