A Molecular Theory for Doubly Resonant IR−UV-vis Sum-Frequency Generation

• DOI: 10.1021/jp012633l
• Publication Date: 2002-07-26T04:49:41Z
• Authors: M. Hayashi; S. H. Lin; M. B. Raschke; Y. R. Shen
• Keywords: Rhodamine 6G; Resonance Raman spectroscopy

The experiment for measuring doubly resonant infrared-visible (IR-vis) sum-frequency generation (SFG) has recently been developed by Shen and his co-worker applied to Rhodamine 6G on silica surfaces. In this paper, based the Born−Oppenheimer adiabatic approximation, a molecular theory IR-vis SFG as two-dimensional surface spectroscopy is presented. We shall show that new nonlinear closely related IR resonance Raman spectroscopy. preliminary theoretical derivation, displaced harmonic potential energy surfaces model electronic ground electronically excited states of system are used obtain band shape functions at finite temperature. One unique powerful abilities interference effects among IR-active modes can be observed. calculated excitation profiles spectra IR−UV from fused demonstrated. provide experimentalists with access microscopic properties molecules or interfaces.