Direct and indirect DIET and DIMET from semiconductor and metal surfaces: What can we learn from ‘toy models’?

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

“…In the vibrational eigenstate basis, hkjðL H þ L D Þqjli gives precisely the left-hand-sides of Eqs. (10) and (11), respectively.rðtÞ is a Lagrange density operator to enforce this second constraint. The variational calculus leads to coupled equations for the field, the density operatorq (obtained by forward propagation), and the Lagrange multiplierr (obtained by backward propagation), which can be solved with an iterative scheme as outlined in greater detail in Refs.…”

“…The IR excitation is direct and controllable, and prepares the system for the subsequent photoreaction. Similar IR + UV/vis strategies to control the photodesorption or other reactions of molecules at surfaces have been suggested elsewhere [8][9][10][11][12][13][14][15][16].…”

Quantum Dynamical Approach to Ultrafast Molecular Desorption from Surfaces

“…In particular, the wave packet hopping scheme of Gadzuk was used for STM-induced desorption in the "above threshold" regime 39,40,[201][202][203] and for ESD. [204][205][206] I will return to some of these later.…”

Computational studies of nonadiabatic effects in gas—surface encounters

“…The desorption of a molecule from a surface induced by electronic transitions is a process involving fundamentally important processes. 1,2 Under the "standard" conditions, 3 the excitation is dominated by single-electron transitions, with excitation energies on the order of a few electron volts, and excited state lifetimes of a few femtoseconds. The desorption probabilities are low, and vibrationally and rotationally state-resolved measurements of the desorption flux show that the internal and translational energies of the desorbates are higher than thermal, but only moderately so.…”