Molecular TennisFlat Smashes and Wicked Cuts

Molecular photodissociation typically produces open-shell photofragments that have angular momentum. This Account explores how the measurement of the directional nature of photofragment angular momentum can provide us with a new viewpoint for seeing and understanding the process whereby molecules fall apart under irradiation. Although the photodissociation process is more complicated than might be imagined at first, the measurements reveal detail that approaches conventional bound-state spectroscopy, enhancing our understanding of the chemical bond and even allowing us to manipulate the ultimate fate of a photofragment by selecting the wavelength and the polarization of the photolysis source.