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Molecular dynamics simulations applied to electric field induced second harmonic generation in dipolar chromophore solutions
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).ORCID iD: 0000-0001-8198-9284
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).ORCID iD: 0000-0003-0007-0394
KTH, School of Biotechnology (BIO), Theoretical Chemistry (closed 20110512).ORCID iD: 0000-0002-1763-9383
2006 (English)In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 110, no 18, 8971-8977 p.Article in journal (Refereed) Published
Abstract [en]

Electric field induced second harmonic generation (EFISH) is an important experimental technique in extracting the first hyperpolarizability of an organic chromophore molecule. Such experiments are carried out in solutions with chromophore molecules dissolved in some common solvents. A known fact is that the first hyperpolarizabilities extracted from EFISH experiments are subject to the use of local field factors. In this work, we apply simulations to study the EFISH properties of chromophore solutions. By combining quantum chemistry calculations with the results derived from molecular dynamics simulations, we show how macroscopic EFISH properties can be modeled, using 4-(dimethylamino)-4'-nitroazobenzene dissolved in chloroform as a demonstration case. The focus of the study is on deriving accurate local field factors. We find that the local field approach applies very well to dipolar solutions, such as the one studied here, but that the local field factors derived are much smaller than the commonly used Onsager or Lorentz local field factors. Our study indicates that many of the reported first hyperpolarizabilities for dipolar molecules from EFISH experiments are most probably underestimated because the Onsager/Lorentz approach, commonly used in extracting the molecular first hyperpolarizability, neglects the effects of the shapes of dipolar chromophore molecules on the local field factors.

Place, publisher, year, edition, pages
2006. Vol. 110, no 18, 8971-8977 p.
Keyword [en]
nonlinear-optical properties, hyper-rayleigh scattering, particle mesh ewald, order hyperpolarizabilities, organic-molecules, polarizabilities, stilbene, polymer, systems, design
National Category
Theoretical Chemistry
URN: urn:nbn:se:kth:diva-15664DOI: 10.1021/jp0603583ISI: 000237451300013ScopusID: 2-s2.0-33744825174OAI: diva2:333706
QC 20100525 QC 20120229Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2012-02-29Bibliographically approved

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Tu, YaoquanLuo, YiÅgren, Hans
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