Rapid motion capture of mode-specific quantum wave packets selectively generated by phase-controlled optical pulses.

Rapid motion capture of phase-controlled wave packets was realized using a sensitive wave-packet spectrometer, which was previously developed by the present authors. Two-dimensional Fourier-transformed spectrograms obtained by the wave-packet spectrometer provide us full information about the wave-packet motion on both excited- and ground-state potential surfaces. Vibrational wave packet associated with a twisting mode in a DTTCI molecule was observed to be dependent on the pulse chirp, and was generated in the excited state preferably with negatively chirped excitation. The result indicates that the excited-state wave packet can be driven along a favorable configuration coordinate by using phase-controlled femtosecond pulses. The present method is essential to adaptive coherent-control application.