Two-Photon-Excited Fluorescence-Encoded Infrared Spectroscopy.
We report on a method for performing ultrafast infrared (IR) vibrational spectroscopy using fluorescence detection. Vibrational dynamics on the ground electronic state driven by femtosecond mid-infrared pulses are detected by changes in fluorescence amplitude resulting from modulation of a two-photon visible transition by nuclear motion. We examine a series of coumarin dyes and study the signals as a function of solvent and excitation pulse parameters. The measured signal characterizes the relaxation of vibrational populations and coherences but yields different information than conventional IR transient absorption measurements. These differences result from the manner in which the ground-state dynamics are projected by the two-photon detection step. Extensions of this method can be adapted for a variety of increased-sensitivity IR measurements.
Department of Chemistry, the James Franck Institute, and the Institute for Biophysical Dynamics University of Chicago , Chicago, Illinois 60637, United States.
Joseph N
JN
Mastron
Department of Chemistry, the James Franck Institute, and the Institute for Biophysical Dynamics University of Chicago , Chicago, Illinois 60637, United States.
Andrei
A
Tokmakoff
D003374:Coumarins / Q000737:chemistry*; D005453:Fluorescence; D017785:Photons; D013050:Spectrometry, Fluorescence / Q000295:instrumentation / Q000379:methods*; D013055:Spectrophotometry, Infrared / Q000295:instrumentation / Q000379:methods*; D014732:Vibration
D003374:Coumarins