Development of high-brightness ultrafast electron microscope for studying nanoscale dynamics associated with strongly correlated materials

Strongly correlated-electron materials are a class of materials that exhibit numerous intriguing emergent phenomena, including metal-to-insulator transition, colossal magnetoresistance, high-temperature superconductivity, etc. These phenomena are beyond the reach of the conventional solid state physics, which is based on the band theory. Instead, strong electron-electron correlations are found to play important roles, which leads to complicated interplay between different degrees of freedoms (charge, lattice, spins...). In this thesis, ultrafast electron diffraction (UED) is used to investigate the photo-induced ultrafast structural dynamics of strongly correlated materials, among which VO2 is taken as an exemplar system, one that reveals the fundamental physics behind photo-induced phase transitions, electron-electron correlation on nanometer scales, and the electron-phonon coupling in this exotic class of materials. The phenomena presented here are expected to have more general significance as they may reflect the physics to which other strongly correlated materials also conform.;In polycrystalline VO2 thin films, the structural changes resulting from photoexcitation with femtosecond laser pulses with different wavelengths are observed to lead to non-thermal phase transitions, which require less energy compared to the phase transitions induced by thermal excitation. The details of the structural change are extracted from the UED results revealing stepwise atomic movements after photoexcitation, which suggests the phase transition starts with a dilation of the correlated d electrons. On the other hand, the structural phase transition is found to be decoupled from the metal-to-insulator transition when the sample dimension is reduced to the sub-micrometer scale, which is attributed to the interface charge doping effects from different substrates. A new phase (M3, monoclinic metallic phase) is distinguished, which has not been discussed by the existing theoretical investigations. The reduction of the optical spectral weight and the anisotropic phononic response is revealed by the UED measurements in the noncooperative phase-transition region, suggesting intriguing interplay between the Mott-Hubbard correlated electrons and the Peierls lattice distortion.;The first-generation UED system is found to be limited by its brightness when high spatiotemporal resolution is required for the studies on nanometer-scale materials. The major constrain on the brightness is the space charge effect, which affects the phase space of the electron pulses. Using the projection-shadow-image technique, the space charge effects in the near-cathode-surface region are investigated. The results suggest a strong space-charge-led perturbation on the electrons' spatial and momentum distributions in the early stage of the short-pulse generation, and the performance with possible corrections in the drift region is discussed under the framework of a mean-field theory.;In laboratory, a radio-frequency (RF) cavity is implemented as a longitudinal focusing lens in the ultrafast electron microscope (UEM). The RF compression together with several magnetic lenses in the beam path, reshapes the electrons' phase space to achieve high brightness and high temporal resolution at the same time. High precision phase-lock between the electron pulses and the RF electric field timing is achieved by implementing a low-level RF phase-locked loop (PLL), an RF-amplifier station and a cavity PLL. The details of these RF systems are introduced, with characterization results presented. The RF-compression UEM is preliminarily characterized, which demonstrates the feasibility of using RF compression to generate high-brightness electron pulses. Future improvements and prospects for the system are also discussed.