The Coulomb explosion method for imaging molecular structure is combined with the femtosecond pump–probe technique. Thus the imaging method becomes flexible enough to determine molecular structure even in highly excited or transient states as a function of time. Examples for the applicability of this method are given. The major concerns which could limit the reliability and the accuracy of the information extracted are discussed and solutions proposed. In addition to observing time–dependent structures, optically triggered Coulomb explosion imaging can be used to identify unusual events in an ensemble of common but more frequent events.
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences356, no. 1736 (15 February 1998): 329–344.