Recently, we presented the detection of carbon monoxide in the transmission spectrum of extrasolar planet HD209458b, using CRIRES, the Cryogenic high-resolution Infrared Echelle Spectrograph at ESO's Very Large Telescope (VLT). The high spectral resolution observations (R=100,000) provide a wealth of information on the planet's orbit, mass, composition, and even on its atmospheric dynamics. The new observational strategy and data analysis techniques open up a whole world of opportunities. We therefore started an ESO large program using CRIRES to explore these, targeting both transiting and non-transiting planets in carbon monoxide, water vapour, and methane. Observations of the latter molecule will also serve as a test-bed for METIS, the proposed mid-infrared imager and spectrograph for the European Extremely Large Telescope.