The observation of the vibrational spectra of adsorbed species provides one of the most incisive methods for und erst an ding chemical and physical phenomena on surfaces. At the present time, many approaches may be applied to studies of molecular vibrations on surfaces. Some of these are used on high-area solids of technological importance (e.g., heterogeneous catalysts) while others are applied to single-crystal substrates to gain better understanding under conditions of controlled surface structure. This book has attempted to bring together in one place a discussion of the major methods used to measure vibrational spectra of surface species. The emphasis is on basic concepts and experimental methods rather than a current survey of the extensive literature in this field. Two introductory chapters describe the basic theoretical aspects of vibrational spectroscopy on surfaces, dealing with normal modes and excitation mechanisms in vibrational spectroscopy. The remaining seven chapters deal with various methods employed to observe surface vibra tions. These are arranged in an order that first treats the use of various methods on surfaces that are not of the single-crystal type. It is in this area that the field first got started in the late 1940s with pioneering work by Terenin and others in the Soviet Union, and by Eisehens and others in the United States in the 1950s. The last four chapters deal with relatively recent methods that permit vibrational studies to be made on single crystal substrates.