Phase modulation of ultrashort light pulses using molecular rotational wave packets

We demonstrate experimentally how the time-dependent phase modulation induced by molecular rotational wave packets can manipulate the phase and spectral content of ultrashort light pulses. Using impulsively excited rotational wave packets in CO2, we increase the bandwidth of a probe pulse by a factor of 9, while inducing a negative chirp. This chirp is removed by propagation through a fused silica window, without the use of a pulse compressor. This is a very general technique for optical phase modulation that can be applied over a broad spectral region from the IR to the UV.