Jie Yang, Markus Gühr, Theodore Vecchione, Matthew Scott Robinson, Renkai Li, Nick Hartmann, Xiaozhe Shen, Ryan Coffee, Jeff Corbett, Alan Fry, Kelly Gaffney, Tais Gorkhover, Carsten Hast, Keith Jobe, Igor Makasyuk, Alexander Reid, Joseph Robinson, Sharon Vetter, Fenglin Wang, Stephen Weathersby, Charles Yoneda, Martin Centurion, Xijie Wang

• Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angstrom spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 angstrom) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.