The anharmonic vibrational ladder of nitric oxide (NO) is climbed by irradiating the molecule with chirped intense (sub)picosecond infrared (IR) pulses (1max=1.0 X 1010 W/cm2). The chirp of the broadband IR (hv = 1850 cm-1, Dhv =50 cm -1) pulse from a free-electron laser is controlled by a pulse shaper. Transfer up to the excited vibrational state X2P1/2(v= 3) of NO shows a strong enhancement when the frequency chirp of the IR pulses follows the consecutive anharmonic vibrational transitions.

Chem. Phys. Lett.

Maas, D. J., Duncan, D. I., Vrijen, R. B., van der Zande, W. J., & Noordam, L. D. (1998). Vibrational ladder climbing in NO by (sub)picosecond frequency-chirped infrared laser pulses. Chem. Phys. Lett., 290, 75–80.