Enhanced Two‐Photon Absorption of Organic Chromophores: Theoretical and Experimental Assessments

Functional organic materials with enhanced two‐photon absorption lead to new technologies in the fields of chemistry, biology, and photonics. In this article we review experimental and theoretical methodologies allowing detailed investigation and analysis of two‐photon absorption properties of organic chromophores. This includes femtosecond two‐photon excited fluorescence experimental setups and quantum‐chemical methodologies based on time‐dependent density functional theory. We thoroughly analyze physical phenomena and trends leading to large two‐photon absorption responses of a few series of model chromophores focusing on the effects of symmetric and asymmetric donor/acceptor substitution and branching.