Molecular “\(\mathit{\pi }\)Pulse” for Total Inversion of Electronic State Population

High-energy 20-fs pulses generated by a Ti:sapphire laser system were spectrally broadened to more than 250 nm by self-phase modulation in a hollow fiber filled with noble gases and subsequently compressed in a broadband high-throughput dispersive system. Pulses as short as 4.5 fs with energy up to 20-microJ were obtained with krypton, while pulses as short as 5 fs with energy up to 70 microJ were obtained with argon. These pulses are, to our knowledge, the shortest generated to date at multigigawatt peak powers.