Journal
CHEMPHYSCHEM
Volume 14, Issue 16, Pages 3731-3739Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201300695
Keywords
absorption; charge transfer; density functional calculations; solvatochromism; solvent effects
Funding
- Foundation for Polish Science under the Welcome program
- Foundation for Polish Science
- Danish Councils for Independent Research
- Villum Foundation
- Lundbeck foundation
- Swedish Infrastructure Committee (SNIC) [SNIC 025/12-38]
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In this study, we report on the influence of solvent on the two-photon absorption (2PA) spectra of Reichardt's dye (RD). The measurement of 2PA cross-sections is performed for three solvents (chloroform, dimethyl formamide, and dimethyl sulfoxide) using the Z-scan technique. The key finding of this study is the observation that the cross-section, corresponding to the 2PA of the intramolecular charge-transfer state, diminishes substantially upon increasing the solvent polarity. To unravel the solvent dependence of the 2PA cross-section, the electronic structure of RD is determined using a hybrid quantum mechanics/molecular mechanics (QM/MM) approach, in which polarization between the solute and solvent is taken into account by using a self-consistent scheme in the solvent polarization. The two-state approximation proves to be adequate for the studied system, and allowed the observed solvent-polarity-induced decrease of the 2PA cross-section to be related to the decrease of the transition moment and the increase in the excitation energy.
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