LAUSR

Significance Excitation of molecules by an ultrashort laser pulse creates rotational wave packets that lead to transient alignment of the molecules along the laser polarization direction. Here, we show that a train of ultrashort laser pulses can be used to enhance the degree of alignment to a high level such that the diffraction from precisely timed ultrashort electron beams may be used to reconstruct the structure of the isolated molecules with atomic resolution through a coherent diffraction imaging technique. Our results mark a great step toward imaging noncrystallized molecules with atomic resolution and pave the way for creation of three-dimensional “molecular movies” at the femtosecond time scale and atomic spatial scale.