We exploit the inherent mode competition in a laser resonator to solve in real time the major coherent control problem — how to shape a pulse that will dump a general wave-packet in to a single target state.
Optical oscillators present a powerful optimization mechanism. The inherent competition for the gain resources between possible modes of oscillation entails the prevalence of the most efficient single mode. We harness this "ultrafast" coherent feedback to optimize an optical field in time, and show that, when an optical oscillator based on a molecular gain medium is synchronously pumped by ultrashort pulses, a temporally coherent multimode field can develop that optimally dumps a general, dynamically evolving vibrational wave packet, into a single vibrational target state. Measuring the emitted field opens a new window to visualization and control of fast molecular dynamics. The realization of such a coherent oscillator with hot alkali dimers appears within experimental reach.
Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic dynamics, they have largely been restricted to ionic systems, with nuclear motion often neglected or indirectly inferred. Here, we demonstrate a ``molecular attoscope", which uses shaped laser pulses in the deep ultraviolet to perform a coherent measurement of electronic and nuclear dynamics in an entangled wave packet in neutral benzene. This enables us to trace both the 856-attosecond-period electronic motion and the 36-femtosecond-period nuclear motion. We observe electronic coherence persisting over hundreds of optical cycles, modulated by nuclear dynamics. Our holographic approach is general, and lays the groundwork for coherent measurements capable of visualizing the evolution of the coupled electronic-nuclear wave function in real time.
Motivated by recent experimental progress achieved with ultracold atoms in kilohertz-driven optical lattices, we provide a theoretical discussion of mechanisms governing the response of a particle in a cosine lattice potential to strong forcing pulses with smooth envelope. Such pulses effectuate adiabatic motion of a wave packet's momentum distribution on quasienergy surfaces created by spatiotemporal Bloch waves. Deviations from adiabaticity can then be deliberately exploited for exerting coherent control and for reaching target states which may not be accessible by other means. As one particular example, we consider an analog of the $\ensuremath{\pi}$ pulses known from optical resonance. We also suggest adapting further techniques previously developed for controlling atomic and molecular dynamics by laser pulses to the coherent control of matter waves in shaken optical lattices.