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Title
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Organic compounds with large and high-contrast pH-switchable nonlinear optical response
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Author
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Abstract
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| Measurements of the nonlinear optical (NLO) response (molecular first hyperpolarizability, beta) of two pH-switchable dyes were performed by means of hyper-Rayleigh scattering (HRS) over a wide range of laser wavelengths and pH values. The extensive wavelength-dependent NLO data combined with linear optical spectroscopy allow the results to be related to the electronic structures of the push-pull systems and the NLO switching contrast to be optimized. The results are modeled theoretically using a vibronic beta dispersion model including both homogeneous and inhomogeneous broadening, yielding a full wavelength dependence of beta, as well as of its switching contrast. The hyperpolarizabilities measured for the basic "on"-states are the highest ever reported for such compounds, reaching over 200 X 10(-30) esu in the static limit and over 2700 X 10(-30) esu at resonance. By combining a high intrinsic contrast in the static hyperpolarizability beta(0) with a large shift in resonance, an extremely large range in contrasts of the HRS signal is reached of more than 2 orders of magnitude at wavelengths accessible with the widely used Ti:sapphire laser and moreover within a biologically compatible pH range. |
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Language
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English
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Source (journal)
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The journal of physical chemistry: C : nanomaterials and interfaces. - Washington, D.C., 2007, currens
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Publication
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Washington, D.C.
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2015
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ISSN
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1932-7447
[print]
1932-7455
[online]
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DOI
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10.1021/ACS.JPCC.5B06968
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Volume/pages
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119
:37
(2015)
, p. 21658-21663
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ISI
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000361868400043
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Full text (Publisher's DOI)
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