The ultrafast vibrational response of hydrogen bonds in the 7-azaindole dimer, a model compound for DNA base pairing, is studied in infrared pump-probe experiments. We observe a similar to 100 fs relaxation of the v = 1 state of the N-H stretching oscillators via anharmonically coupled over- and combination tones of fingerprint modes. In the monomer with a larger energy mismatch between the v = I state and over-/combination tones, a much longer lifetime of 10 ps is found. Ferntosecond N-H stretching excitation induces coherent underdamped motions of the dimer, dominated by the anharmonically coupled 110 cm(-1) stretching mode of the hydrogen bonds. (c) 2006 Elsevier B.V. All rights reserved.