Abstract
This chapter provides selected examples of experimental investigations addressing the role of rotational and vibrational energy in adsorption at surfaces. Such information can generally be obtained in different ways characterized by different degrees of state selectivity. The first part of the chapter deals with the effect of rotational energy, while the second considers the effect of vibrational energy. The former investigations compared the behavior of rotationally hot and cold molecular beams by measuring the sticking probability on well-defined surfaces under controlled, ultrahigh-vacuum conditions. When detection of the rotational state of gas-phase molecules became feasible, a large amount of information was obtained indirectly: researchers first determined experimentally the rotational state of desorbing (or scattered) molecules and then used microreversibility (otherwise called detailed balance) arguments to extract information on the effect of the rotational states on the sticking probability. In recent years, methods to prepare molecules in partially and, in some cases, even fully defined rotational quantum states were developed. The central part of the section highlights recent results obtained using electrostatic and finally magnetic hexapoles. The first section of the chapter ends by reviewing results obtained by exploiting the velocity dependence of the degree of alignment of molecules seeded with inert carriers in a supersonic molecular beam. A brief selection of resultsobtained with laser methods concludes this section. Laser methods are on the contrary indispensable for the preparation of vibrationally excited molecules, which is the topic of the second section of the chapter. The relative roles of kinetic and vibrational energy are discussed, and the concepts of entrance and late barrier in the potential energy surface are introduced. Pioneering experiments showing greater specificity in surface reactions are briefly reviewed.
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Vattuone, L., Okada, M. (2020). State Resolved Sticking Probability in Gas-Surface Interaction. In: Rocca, M., Rahman, T.S., Vattuone, L. (eds) Springer Handbook of Surface Science. Springer Handbooks. Springer, Cham. https://doi.org/10.1007/978-3-030-46906-1_32
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