Fig. 1: Schematic structure, experimental setup, and Ewald sphere.

a Molecular structure of the complex 1 in the LS state. Black balls are carbon atoms; blue balls are nitrogen atoms; brown balls are iron atoms; purple balls are boron atoms; pink balls are hydrogen atoms; b Unit-cell and molecular structure of 1 in the LT (T = 300 K) (blue bonds and unit-cell edges) and HT (T = 373 K) (red bonds and unit-cell edges) phases. Hydrogen atoms are omitted for clarity. c Schematic of the experimental setup and representative diffraction images. After photoexcitation with 267-nm pump pulses, the structural response of 1 was measured separately by (i) ultrafast XRD at an XFEL and (ii) MeV-UED. d Construction of the Ewald sphere for the XFEL (red) and MeV UED (green) experiments. The specific energies of the keV XFEL and MeV electron sources imply vastly different radii of the Ewald spheres for the XRD and UED experiments, respectively.