Ultrafast electron diffraction (UED) is a powerful technique that can be used to resolve structural changes of gas molecules during a photochemical reaction. However, the temporal resolution in pump-probe experiments has been limited to the few-ps level by the space-charge effect that broadens the electron pulse duration and by velocity mismatch between the pump laser pulses and the probe electron pulses, making only long-lived intermediate states accessible. Taking advantage of relativistic effects, Mega-electron-volt (MeV) electrons can be used to suppress both the space-charge effect and the velocity mismatch, and hence to achieve a temporal resolution that is fast enough to follow coherent nuclear motion in the target molecules. In this presentation, we show the first MeV UED experiments on gas phase targets. These experiments not only demonstrate that femtosecond temporal resolution is achieved, but also show that the spatial resolution is not compromised. This unprecedented combination of spatiotemporal resolution is sufficient to image coherent nuclear motions, and opens the door to a new class of experiments where the structural changes can be followed simultaneously in both space and time.
A two-step algorithm is developed that can reconstruct the full 3-D molecular structure from diffraction patterns of
partially aligned molecules in gas phase. This method is applicable to asymmetric-top molecules that do not need to have
any specific symmetry. This method will be important for studying dynamical processes that involve transient structures
where symmetries, if any, can possibly be broken. A new setup for the diffraction experiments that can provide enough
time resolution as well as high currents suitable for gas phase experiments is reported. Time resolution is obtained by
longitudinal compression of electron pulses by time-varying electric fields synchronized to the motion of electron pulses.