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651641 
Journal Article 
Time-resolved molecular frame dynamics of fixed-in-space CS2 molecules 
Bisgaard, CZ; Clarkin, OJ; Wu, G; Lee, AM; Gessner, O; Hayden, CC; Stolow, A 
2009 
Science
ISSN: 0036-8075
EISSN: 1095-9203 
323 
5920 
1464-1468 
English 
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.