How to realize an ultrafast electron diffraction experiment with a terahertz pump: a theoretical study

To integrate a terahertz pump into an ultrafast electron diffraction (UED) experiment has attracted much attention due to its potential to initiate and detect the structural dynamics both directly. However, the deflection of the electron probe by the electromagnetic field of the terahertz pump alters the incident angle of the electron probe on the sample, impeding it from recording structural information afterwards. In this article, we studied this issue by a theoretical simulation of the terahertz-induced deflection effect on the electron probe, and came up with several possible schemes to reduce such effect. As a result, a terahertz-pump-electron-probe UED experiment with a temporal resolution comparable to the terahertz period is realized. We also found that MeV UED was more suitable for such terahertz pump experiment.

Overview of the Semiconductor Photocathode Research in China

With the growing demand from scientific projects such as the X-ray free electron laser (XFEL), ultrafast electron diffraction/microscopy (UED/UEM) and electron ion collider (EIC), the semiconductor photocathode, which is a key technique for a high brightness electron source, has been widely studied in China. Several fabrication systems have been designed and constructed in different institutes and the vacuum of most systems is in the low 10−8 Pa level to grow a high QE and long lifetime photocathode. The QE, dark lifetime/bunch lifetime, spectral response and QE map of photocathodes with different kinds of materials, such as bialkali (K2CsSb, K2NaSb, etc.), Cs2Te and GaAs, have been investigated. These photocathodes will be used to deliver electron beams in a high voltage DC gun, a normal conducting RF gun, and an SRF gun. The emission physics of the semiconductor photocathode and intrinsic emittance reduction are also studied.

Ultrafast Imaging of Molecules with Electron Diffraction

Photoexcited molecules convert light into chemical and mechanical energy through changes in electronic and nuclear structure that take place on femtosecond timescales. Gas phase ultrafast electron diffraction (GUED) is an ideal tool to probe the nuclear geometry evolution of the molecules and complements spectroscopic methods that are mostly sensitive to the electronic state. GUED is a passive probing tool that does not alter the molecular properties during the probing process and is sensitive to the spatial distribution of charge in the molecule, including both electrons and nuclei. Improvements in temporal resolution have enabled GUED to capture coherent nuclear motions in molecules in the excited and ground electronic states with femtosecond and subangstrom resolution. Here we present the basic theory of GUED and explain what information is encoded in the diffraction signal, review how GUED has been used to observe coherent structural dynamics in recent experiments, and discuss the advantages and limitations of the method. Expected final online publication date for the Annual Review of Physical Chemistry, Volume 73 is April 2022. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.

Quantum state tomography of molecules by ultrafast diffraction

Ultrafast electron diffraction and time-resolved serial crystallography are the basis of the ongoing revolution in capturing at the atomic level of detail the structural dynamics of molecules. However, most experiments capture only the probability density of the nuclear wavepackets to determine the time-dependent molecular structures, while the full quantum state has not been accessed. Here, we introduce a framework for the preparation and ultrafast coherent diffraction from rotational wave packets of molecules, and we establish a new variant of quantum state tomography for ultrafast electron diffraction to characterize the molecular quantum states. The ability to reconstruct the density matrix, which encodes the amplitude and phase of the wavepacket, for molecules of arbitrary degrees of freedom, will enable the reconstruction of a quantum molecular movie from experimental x-ray or electron diffraction data.