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The measurement of 2PA cross\u2010sections is performed for three solvents (chloroform, dimethyl formamide, and dimethyl sulfoxide) using the <jats:italic>Z<\/jats:italic>\u2010scan technique. The key finding of this study is the observation that the cross\u2010section, corresponding to the 2PA of the intramolecular charge\u2010transfer state, diminishes substantially upon increasing the solvent polarity. To unravel the solvent dependence of the 2PA cross\u2010section, 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\u2010consistent scheme in the solvent polarization. The two\u2010state approximation proves to be adequate for the studied system, and allowed the observed solvent\u2010polarity\u2010induced decrease of the 2PA cross\u2010section to be related to the decrease of the transition moment and the increase in the excitation energy.<\/jats:p>","DOI":"10.1002\/cphc.201300695","type":"journal-article","created":{"date-parts":[[2013,10,4]],"date-time":"2013-10-04T06:03:32Z","timestamp":1380866612000},"page":"3731-3739","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":40,"title":["Two\u2010Photon Solvatochromism II: Experimental and Theoretical Study of Solvent Effects on the Two\u2010Photon Absorption Spectrum of Reichardt\u2019s Dye"],"prefix":"10.1002","volume":"14","author":[{"given":"Ma\u0142gorzata","family":"Wielgus","sequence":"first","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Robert","family":"Zale\u015bny","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"N. 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