Publications of this research are reported in Science, JACS, JPC, ChemPhysChem, PNAS, Nano Lett., and PCCP. Developmentally, we have advanced ultrafast electron microscopy (and diffraction) to a new level. The electron pulses typically have an energy of 30 keV for diffraction and 100-200 keV for microscopy, corresponding to speeds of 33-70% of the speed of light. Recently, we introduced the concept of tilted optical pulses into diffraction and imaging techniques and demonstrated the methodology experimentally. In a separate contribution, we provided a novel approach for reaching the attosecond time domain. Such attosecond electron pulses are significantly shorter than those achievable with extreme UV light sources near 25 nm (-50 eV) and have the potential for applications in the visualization of ultrafast electron dynamics.