Development of ultrafast four-dimensional precession electron diffraction

Ultrafast electron diffraction/microscopy technique enables us to investigate the nonequilibrium dynamics of crystal structures in the femtosecond-nanosecond time domain. However, the electron diffraction intensities are in general extremely sensitive to the excitation errors (i.e., deviation from the Bragg condition) and the dynamical effects, which had prevented us from quantitatively discussing the crystal structure dynamics particularly in thick samples. Here, we develop a four-dimensional precession electron diffraction (4D-PED) system by which time (t) and electron-incident-angle $\left(\varphi \right)$ dependences of electron diffraction patterns $\left(q_x,q_y\right)$ are recorded. Nonequilibrium crystal structure refinement on VTe₂ demonstrates that the ultrafast change in the crystal structure can be quantitatively determined from 4D-PED. We further perform the analysis of the $\varphi$ dependence, from which we can qualitatively estimate the change in the reciprocal lattice vector parallel to the optical axis. These results show the capability of the 4D-PED method for the quantitative investigation of ultrafast crystal structural dynamics.