title: 'Making the molecular movie': first frames.
abstract: Recent advances in high-intensity electron and X-ray pulsed sources now make it possible to directly observe atomic motions as they occur in barrier-crossing processes. These rare events require the structural dynamics to be triggered by femtosecond excitation pulses that prepare the system above the barrier or access new potential energy surfaces that drive the structural changes. In general, the sampling process modifies the system such that the structural probes should ideally have sufficient intensity to fully resolve structures near the single-shot limit for a given time point. New developments in both source intensity and temporal characterization of the pulsed sampling mode have made it possible to make so-called 'molecular movies', i.e. measure relative atomic motions faster than collisions can blur information on correlations. Strongly driven phase transitions from thermally propagated melting to optically modified potential energy surfaces leading to ballistic phase transitions and bond stiffening are given as examples of the new insights that can be gained from an atomic level perspective of structural dynamics. The most important impact will likely be made in the fields of chemistry and biology where the central unifying concept of the transition state will come under direct observation and enable a reduction of high-dimensional complex reaction surfaces to the key reactive modes, as long mastered by Mother Nature.
authors.affiliation: Department of Chemistry, and Institute for Optical Sciences, University of Toronto, 80 St George Street, Toronto, Ontario, Canada M5S 3H6. dmiller@lphys.chem.utoronto.ca
authors.forename: R J Dwayne
authors.initials: RJ
authors.lastname: Miller
authors.forename: Ralph
authors.initials: R
authors.lastname: Ernstorfer
authors.forename: Maher
authors.initials: M
authors.lastname: Harb
authors.forename: Meng
authors.initials: M
authors.lastname: Gao
authors.forename: Christoph T
authors.initials: CT
authors.lastname: Hebeisen
authors.forename: Hubert
authors.initials: H
authors.lastname: Jean-Ruel
authors.forename: Cheng
authors.initials: C
authors.lastname: Lu
authors.forename: Gustavo
authors.initials: G
authors.lastname: Moriena
authors.forename: German
authors.initials: G
authors.lastname: Sciaini