| Coherent control of chemical reactions, atomic and molecular systems, lattice dynamics, and electronic motion rely on femtosecond laser sources capable of producing programmable arbitrarily shaped waveforms. To enter the time scale of natural dynamic processes in many systems, femtosecond pulse shaping techniques must be extended to the ultrashort pulse domain (<50 fs). Concurrently, reliable high-fidelity amplification of shaped waveforms is required in many applications. We demonstrate ultrabroad bandwidth pulse shaping of 13 fs pulses with Fourier-domain phase-only filtering using a liquid crystal array. We further demonstrate the amplification of shaped pulses in a multipass chirped pulse amplifier (CPA) system to produce millijoule-level optical waveforms with 30 fs resolution.; Recently, a new approach to coherent control of physical systems was introduced, which, instead of relying on formidable theoretical calculations of complex system dynamics, makes use of an appropriate experimental feedback from the system itself to control its evolution. We apply this adaptive feedback approach for enhancement of ionization rates in a femtosecond plasma with the goal of minimization of phase distortions in the amplifier system. With the help of a learning algorithm and survival principles of nature, we teach our laser to control its own phase by using spectral blueshifting in a rapidly created plasma as a feedback to the algorithm.; Control of lattice vibrations has long been sought as a means of studying phonon-related processes in solids. In addition, generation and control of large-amplitude optical phonon modes may open a path to femtosecond time-resolved studies of structural phase transitions and production of ultrashort shaped X-ray pulses. We perform pump-probe phase-resolved measurements and control of optical A1g mode in sapphire through shaped-pulse impulsive stimulated Raman scattering (ISRS). We chose this material as a candidate for possible nonlinear oscillations regime for its wide band gap and superior optical properties allowing for high-energy excitation. To enter a nonlinear regime, however, complex asymmetric multiple-pulse excitation is required. Therefore, we make a detailed proposal of the experimental adaptive feedback implementation for optimization of phonon amplitude based on the coherent probe scattering and a novel phase mask calculation algorithm for the real-time asymmetric pulse train generation. |
