Time- vs. frequency-domain femtosecond surface sum frequency generation
Abstract
We present an experimental and theoretical investigation into time- vs. frequency-domain femtosecond sum frequency spectroscopy at the metal-liquid interface. Although frequency and time-domain measurements are theoretically equivalent it is demonstrated here experimentally that the two approaches are sensitive to different physical aspects of the system and provide complementary information. Time-domain measurements are demonstrated to be more clearly influenced by the inhomogeneity of adsorption sites, since the decay of the vibrational polarization can be mapped directly. A generalization of existing models allows for the simultaneous description of both frequency and time-domain measurements.
- Publication:
-
Chemical Physics Letters
- Pub Date:
- March 2003
- DOI:
- 10.1016/S0009-2614(03)00085-X
- Bibcode:
- 2003CPL...370..227R