Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules
Christer Z. Bisgaard,1
Owen J. Clarkin,1,2
Guorong Wu,1
Anthony M. D. Lee,1,2*
Oliver Geßner,3
Carl C. Hayden,4
Albert Stolow1,2
Random orientation of molecules within a sample leads to blurred
observations of chemical reactions studied from the laboratory
perspective. Methods developed for the dynamic imaging of molecular
structures and processes struggle with this, as measurements
are optimally made in the molecular frame. We used laser alignment
to transiently fix carbon disulfide molecules in space long
enough to elucidate, in the molecular reference frame, details
of ultrafast electronic-vibrational dynamics during a photochemical
reaction. These three-dimensional photoelectron imaging results,
combined with ongoing efforts in molecular alignment and orientation,
presage a wide range of insights obtainable from time-resolved
studies in the molecular frame.
2 Department of Chemistry, Queen's University, Kingston, Ontario K7L 3N6, Canada.
3 Chemical Sciences Division, Lawrence Berkeley National Laboratory, One Cyclotron Road, M/S 2-300, Berkeley, CA 94720, USA.
4 Combustion Research Facility, Sandia National Laboratory, Livermore, CA 94551, USA.
* Present address: Department of Cancer Imaging, BC Cancer Research Centre, Vancouver, British Columbia V5Z 1L3, Canada.
To whom correspondence should be addressed. E-mail: albert.stolow{at}nrc.ca
