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Fourier Transform Fluorescence-Encoded Infrared Spectroscopy.

Joseph N Mastron1, Andrei Tokmakoff1

  • 1Department of Chemistry, The James Franck Institute, and the Institute for Biophysical Dynamics, University of Chicago , Chicago, Illinois 60637, United States.

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|December 19, 2017
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Fourier transform Fluorescence-Encoded Infrared (FEIR) spectroscopy offers high-sensitivity vibrational analysis. This method enables detailed study of coupled vibrations and their dynamics at low concentrations.

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Area of Science:

  • Chemical Physics
  • Spectroscopy

Background:

  • Time-resolved infrared (IR) vibrational spectroscopy is crucial for studying structural dynamics.
  • Current IR techniques are limited to high concentrations, hindering analysis of dilute systems.

Purpose of the Study:

  • To develop Fourier transform Fluorescence-Encoded Infrared (FEIR) spectroscopy for high-sensitivity IR analysis.
  • To enable the study of coupled vibrations and their dynamics at lower concentrations.

Main Methods:

  • Utilizing a pair of IR fields with variable time delay to drive vibrational excitation.
  • Encoding IR-driven excitations into fluorescing excited electronic states.
  • Applying Fourier transformation to interferometric components in encoded fluorescence for spectral analysis.
  • Varying time delays to observe frequency-difference oscillations and construct 2D correlation spectra.

Main Results:

  • Demonstrated Fourier transform FEIR as a high-sensitivity IR spectroscopy technique.
  • Observed interferometric components in encoded fluorescence upon IR excitation.
  • Successfully constructed 2D correlation spectra of coupled vibrations by analyzing frequency-difference oscillations.
  • Modeled response functions that reproduce spectral features and excitation pathways.

Conclusions:

  • Fourier transform FEIR provides a sensitive method for vibrational spectroscopy.
  • The technique allows for the investigation of coupled vibrational dynamics.
  • Observed spectral features correlate to vibrational population and coherence excitation pathways.