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High-resolution electron energy loss spectroscopy and theoretical calculations of related isolated molecules have been used to identify and assign negative ion resonances (NIR) in the vibrational excitation functions of hydrogen and diethylsilane adsorbed on Si(100)-(2x1). For H/Si(100) the NIR at ~3 eV leads to mode selective enhancement of Si-H stretching vibrations. For diethylsilane adsorbed on...