Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Lasers, and Electron Pulses.

The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, X-ray, and electron sources have enabled the direct imaging of evolving molecular structures in chemical processes, and recent experimental advances in preparing ultrafast laser and electron pulses resulted in molecular imaging with femtosecond time resolution. This Perspective presents an overview of the versatile imaging methods of molecular dynamics. High-order harmonic generation imaging and photoelectron diffraction imaging are based on laser-induced ionization and rescattering processes. Coulomb explosion imaging retrieves molecular structural information by detecting the momentum vectors of fragmented ions. Diffraction imaging encodes molecular structural and electronic information in reciprocal space. We also present various applications of these ultrafast imaging methods in resolving laser-induced nuclear and electronic dynamics.