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dc.contributor.author Hu, X
dc.contributor.author Xiao, D
dc.contributor.author Keinan, S
dc.contributor.author Asselberghs, I
dc.contributor.author Therien, MJ
dc.contributor.author Clays, K
dc.contributor.author Yang, W
dc.contributor.author Beratan, DN
dc.date.accessioned 2011-06-21T17:26:44Z
dc.date.issued 2010-02-11
dc.identifier.citation Journal of Physical Chemistry C, 2010, 114 (5), pp. 2349 - 2359
dc.identifier.issn 1932-7447
dc.identifier.uri http://hdl.handle.net/10161/4078
dc.description.abstract Successfully predicting the frequency dispersion of electronic hyperpolarizabilities is an unresolved challenge in materials science and electronic structure theory. We show that the generalized Thomas-Kuhn sum rules, combined with linear absorption data and measured hyperpolarizability at one or two frequencies, may be used to predict the entire frequency-dependent electronic hyperpolarizability spectrum. This treatment includes two- and three-level contributions that arise from the lowest two or three excited electronic state manifolds, enabling us to describe the unusual observed frequency dispersion of the dynamic hyperpolarizability in high oscillator strength M-PZn chromophores, where (porphinato)zinc(II) (PZn) and metal(II)polypyridyl (M) units are connected via an ethyne unit that aligns the high oscillator strength transition dipoles of these components in a head-to-tail arrangement. We show that some of these structures can possess very similar linear absorption spectra yet manifest dramatically different frequency dependent hyperpolarizabilities, because of three-level contributions that result from excited state-to excited state transition dipoles among charge polarized states. Importantly, this approach provides a quantitative scheme to use linear optical absorption spectra and very limited individual hyperpolarizability measurements to predict the entire frequency-dependent nonlinear optical response. Copyright © 2010 American Chemical Society.
dc.format.extent 2349 - 2359
dc.language.iso en_US en_US
dc.relation.ispartof Journal of Physical Chemistry C
dc.relation.isversionof 10.1021/jp911556x
dc.title Predicting the frequency dispersion of electronic hyperpolarizabilities on the basis of absorption data and thomas-kuhn sum rules
dc.title.alternative en_US
dc.type Journal Article
dc.description.version Version of Record en_US
duke.date.pubdate 2010-2-11 en_US
duke.description.endpage 2359 en_US
duke.description.issue 5 en_US
duke.description.startpage 2349 en_US
duke.description.volume 114 en_US
dc.relation.journal Journal of Physical Chemistry C en_US
pubs.issue 5
pubs.organisational-group /Duke
pubs.organisational-group /Duke/Institutes and Provost's Academic Units
pubs.organisational-group /Duke/Institutes and Provost's Academic Units/Initiatives
pubs.organisational-group /Duke/Institutes and Provost's Academic Units/Initiatives/Energy Initiative
pubs.organisational-group /Duke/Pratt School of Engineering
pubs.organisational-group /Duke/Pratt School of Engineering/Biomedical Engineering
pubs.organisational-group /Duke/School of Medicine
pubs.organisational-group /Duke/School of Medicine/Basic Science Departments
pubs.organisational-group /Duke/School of Medicine/Basic Science Departments/Biochemistry
pubs.organisational-group /Duke/School of Medicine/Institutes and Centers
pubs.organisational-group /Duke/School of Medicine/Institutes and Centers/Duke Cancer Institute
pubs.organisational-group /Duke/Trinity College of Arts & Sciences
pubs.organisational-group /Duke/Trinity College of Arts & Sciences/Chemistry
pubs.organisational-group /Duke/Trinity College of Arts & Sciences/Physics
pubs.publication-status Published
pubs.volume 114
dc.identifier.eissn 1932-7455

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