Femtosecond multidimensional imaging of a molecular dissociation.
The coupled electronic and vibrational motions governing chemical processes are best viewed from the molecule's point of view-the molecular frame. Measurements made in the laboratory frame often conceal information because of the random orientations the molecule can take. We used a combination of time-resolved photoelectron spectroscopy, multidimensional coincidence imaging spectroscopy, and ab initio computation to trace a complete reactant-to-product pathway-the photodissociation of the nitric oxide dimer-from the molecule's point of view, on the femtosecond time scale. This method revealed an elusive photochemical process involving intermediate electronic configurations.
Gessner
O
O
Steacie Institute for Molecular Sciences, National Research Council Canada, Ottawa, Ontario K1A 0R6, Canada.
Lee
A M D
AM
Shaffer
J P
JP
Reisler
H
H
Levchenko
S V
SV
Krylov
A I
AI
Underwood
Jonathan G
JG
Shi
H
H
East
A L L
AL
Wardlaw
D M
DM
Chrysostom
E T H
ET
Hayden
C C
CC
Stolow
Albert
A