In many physical and biological systems the transition from an amorphous to ordered native structure involves complex energy landscapes, and understanding such transformations requires not only their thermodynamics but also the structural dynamics during the process. Here, we extend our 4D visualization method with electron imaging to include the study of irreversible processes with a single pulse in the same ultrafast electron microscope (UEM) as used before in the single-electron mode for the study of reversible processes. With this augmentation, we report on the transformation of amorphous to crystalline structure with silicon as an example. A single heating pulse was used to initiate crystallization from the amorphous phase while a single packet of electrons imaged selectively in space the transformation as the structure continuously changes with time. From the evolution of crystallinity in real time and the changes in morphology, for nanosecond and femtosecond pulse heating, we describe two types of processes, one that occurs at early time and involves a nondiffusive motion and another that takes place on a longer time scale. Similar mechanisms of two distinct time scales may perhaps be important in biomolecular folding.diffraction ͉ imaging ͉ structural dynamics ͉ ultrafast electron microscopy T he transformation of amorphous structures, such as liquids or random-coiled proteins, into ordered structures involves complex dynamical processes that ultimately lead to the final native state. The mechanism is determined by the scales of time, length, and energy as they define the nature of the elementary steps involved. For example, an amorphous bulk liquid crystallizes depending on the degree of initial (nanoscale) nucleation, the time scale of heat diffusion, and the latent energy acquired. Similarly, for a protein, the funneling toward the native structure requires the balance of the entropic and enthalpic free energy contributions, as well as the ''diffusion'' through many energy barriers, possibly with nucleation on the path to the final state.To observe such processes on the time-length scale of the phenomena, our method of choice has been 4D space-time visualization (ref. 1 and references therein, and ref. 2) developed in ultrafast electron microscopy (UEM) and diffraction for imaging with a wide scope (3) of applications (1-10). For microscopy, the concept of femtosecond single (or few) electron packets was introduced to allow for the study of structural dynamics in the temporal, space-charge-free regime and to obtain the atomic-scale spatial resolution. In this mode of UEM operation, a train of electron packets coherently ''builds up'' and coheres into the final image. However, for nonequilibrium irreversible processes, such as crystallization, the transformation must be visualized through single-pulse imaging.In this contribution, we augment the UEM apparatus to include this single-pulse capability, thus covering domains of femtoseconds (fs) to seconds. Using this mode of imaging, here reported is the ...