Third‐harmonic generation (THG) with a two‐photon‐absorption (TPA) type resonance was used to monitor the J‐aggregation of ethyl thiacarbocyanine in aqueous solution. Correlations between TPA‐resonant THG and two‐photon‐excited photoluminescence are revealed, indicating the significance of excited states for non‐linear‐optical processes in J‐aggregating solutions. Similar to Raman resonances in coherent anti‐Stokes Raman scattering, TPA resonances in THG allow THG enhancement to be effectively decoupled from the growth of radiation losses.
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Akimov et al. (2003) studied this question.
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