Abstract
Theoretical expressions for sum-frequency generation (SFG) signals, which can be applied to treat various SFG experiments, have been derived. We have applied the theoretical results to study the SFG experiments for the near-electronic resonant, singly resonant IR−UV, and doubly resonant IR−UV cases that are associated with the measurements reported by Shen's group. We have taken into account both the electric and magnetic dipole interactions and the applied laser and detection polarization combinations explicitly. Relationships between the polarization combinations and the electric-dipole−electric-dipole mechanism, the electric-dipole−magnetic-dipole mechanism, the magnetic-dipole−electric-dipole mechanism, and the magnetic-dipole−magnetic-dipole mechanisms are clarified. Based on the theoretical results, near-electronic resonant SFG, singly resonant IR−UV SFG, doubly resonant IR SFG experiments are discussed.
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