Over many millennia, humankind has thought to explore phenomena on an ever shorter time scale. In this race against time, femtosecond resolution (1 fs=10(-15) s) is the ultimate achievement for studies of the fundamental dynamics of the chemical bond. Observation of the very act that brings about chemistry-the making and breaking of bonds on their actual time and length scales-is the wellspring of the field of femtochemistry, which is the study of molecular motions in the hitherto unobserved ephemeral transition states of physical, chemical, and biological changes. For molecular dynamics, achieving this atomic-scale resolution using ultrafast lasers as strobes is a triumph, just as X-ray and electron diffraction, and, more recently, STM and NMR spectroscopy, provided that resolution for static molecular structures. On the femtosecond time scale, matter wave packets (particle-type) can be created and their coherent evolution as a single-molecule trajectory can be observed. The field began with simple systems of a few atoms and has reached the realm of the very complex in isolated, mesoscopic, and condensed phases, as well as in biological systems such as proteins and DNA structures. It also offers new possibilities for the control of reactivity and for structural femtochemistry and femtobiology. This anthology gives an overview of the development of the field from a personal perspective, encompassing our research at Caltech and focusing on the evolution of techniques, concepts, and new discoveries.