Vibrational energy transfer in collisions of molecules with metal surfaces

Igor Rahinov, Alexander Kandratsenka, Tim Schäfer, Pranav Shirhatti, Kai Golibrzuch, Alec M. Wodtke

نتاج البحث: نشر في مجلةمقالة مرجعية مراجعة النظراء

ملخص

The Born-Oppenheimer approximation (BOA), which serves as the basis for our understanding of chemical bonding, reactivity and dynamics, is routinely violated for vibrationally inelastic scattering of molecules at metal surfaces. The title-field therefore represents a fascinating challenge to our conventional wisdom calling for new concepts that involve explicit electron dynamics occurring in concert with nuclear motion. Here, we review progress made in this field over the last decade, which has witnessed dramatic advances in experimental methods, thereby providing a much more extensive set of diverse observations than has ever before been available. We first review the experimental methods used in this field and then provide a systematic tour of the vast array of observations that are currently available. We show how these observations - taken together and without reference to computational simulations - lead us to a simple and intuitive picture of BOA failure in molecular dynamics at metal surfaces, one where electron transfer between the molecule and the metal plays a preeminent role. We also review recent progress made in the theory of electron transfer mediated BOA failure in molecule-surface interactions, describing the most important methods and their ability to reproduce experimental observation. Finally, we outline future directions for research and important unanswered questions.

اللغة الأصليةالإنجليزيّة
الصفحات (من إلى)15090-15114
عدد الصفحات25
دوريةPhysical Chemistry Chemical Physics
مستوى الصوت26
رقم الإصدار21
المعرِّفات الرقمية للأشياء
حالة النشرنُشِر - 29 مايو 2024

ملاحظة ببليوغرافية

Publisher Copyright:
© 2024 The Royal Society of Chemistry.

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