Femtosecond electronic and hydrogen structural dynamics in ammonia imaged with ultrafast electron diffraction


Elio G. Champenois, Nanna H. List, Matthew Ware, Mathew Britton, Philip H. Bucksbaum, Xinxin Cheng, Martin Centurion, James P. Cryan, Ruaridh Forbes, Ian Gabalski, Kareem Hegazy, Matthias C. Hoffmann, Andrew J. Howard, Fuhao Ji, Ming-Fu Lin, J. Pedro F. Nunes, Xiaozhe Shen, Jie Yang, Xijie Wang, Todd J. Martinez, Thomas J. A. Wolf

Phys. Rev. Lett. 131, 143001 (2023)

Directly imaging structural dynamics involving hydrogen atoms by ultrafast diffraction methods is complicated by their low scattering cross sections. Here we demonstrate that megaelectronvolt ultrafast electron diffraction is sufficiently sensitive to follow hydrogen dynamics in isolated molecules. In a study of the photodissociation of gas phase ammonia, we simultaneously observe signatures of the nuclear and corresponding electronic structure changes resulting from the dissociation dynamics in the time-dependent diffraction. Both assignments are confirmed by ab initio simulations of the photochemical dynamics and the resulting diffraction observable. While the temporal resolution of the experiment is insufficient to resolve the dissociation in time, our results represent an important step towards the observation of proton dynamics in real space and time.