We describe a new apparatus that combines pulsed laser excitation in a molecular beam with surface-science methods for preparation of clean single-crystal surfaces and detection of adsorbates to enable state-selected studies of gas-surface reaction dynamics. Reactant molecules are prepared in specific vibrationally excited states via overtone pumping using tunable, narrow-band laser radiation. The collision-free environment of the molecular beam prevents relaxation of the prepared molecules before impact on the target surface and enables complete control over the collision energy and incidence angle. Chemisorption products are detected after a given deposition time by Auger electron spectroscopy. To achieve sufficient beam flux of state-selected reactant molecules for product detection by standard surface-science techniques, we use a high-intensity, short-pulse molecular-beam source matched to the low duty cycle of the pulsed lasers used in our experiments. We present the design and characterization of this new apparatus together with a scheme for generating infrared laser pulses of high spectral brightness for saturating weak vibrational overtone transitions within a significant volume of the molecular beam. The effectiveness of our approach is demonstrated by state-resolved sticking coefficient measurements for overtone-excited (2nu(3)) CH4 on Ni(100) for a range of impact energies. (C) 2003 American Institute of Physics.