Controlling the non-resonant chemical mechanism of SERS using a molecular photoswitch
Identifieur interne : 000C27 ( Main/Exploration ); précédent : 000C26; suivant : 000C28Controlling the non-resonant chemical mechanism of SERS using a molecular photoswitch
Auteurs : Seth Michael Morton [États-Unis] ; Ebo Ewusi-Annan [États-Unis] ; Lasse Jensen [États-Unis]Source :
- Physical Chemistry Chemical Physics [ 1463-9076 ] ; 2009.
Abstract
In this work we present a detailed investigation of the Raman properties of a dithienylethene photoswitch interacting with a small gold cluster (Au19+) using time-dependent density functional theory (TD-DFT). The enhancement mechanism (CHEM) due to the moleculesurface chemical coupling in surface-enhanced Raman scattering (SERS) has been characterized for this system. We demonstrate that it is possible to control the CHEM enhancement by switching the photoswitch from its closed form to its open form. The open form of the photoswitch is found to be the strongest Raman scatterer when adsorbed on the surface whereas the opposite is found for the free molecule. This trend is explained using a simple two-state approximation. In this model the CHEM enhancement scales roughly as (X/e)4, where X is the HOMOLUMO gap of the free molecule and e is an average excitation between the HOMO of the photoswitch and the LUMO of the metal. We propose that the ability of this photoswitch to switch reversibly from open to closed will make it an excellent probe to control the CHEM enhancement of SERS.
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DOI: 10.1039/b904745j
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Chem. Chem. Phys.</title><idno type="ISSN">1463-9076</idno><idno type="eISSN">1463-9084</idno><imprint><publisher>The Royal Society of Chemistry.</publisher><date type="published" when="2009">2009</date><biblScope unit="volume"></biblScope><biblScope unit="issue">34</biblScope><biblScope unit="page" from="7424">7424</biblScope><biblScope unit="page" to="7429">7429</biblScope></imprint><idno type="ISSN">1463-9076</idno></series><idno type="istex">82597F292BC5CCB4738C4F0665642DD8B7805A46</idno><idno type="DOI">10.1039/b904745j</idno><idno type="ms-id">b904745j</idno></biblStruct></sourceDesc><seriesStmt><idno type="ISSN">1463-9076</idno></seriesStmt></fileDesc><profileDesc><textClass></textClass><langUsage><language ident="en">en</language></langUsage></profileDesc></teiHeader><front><div type="abstract">In this work we present a detailed investigation of the Raman properties of a dithienylethene photoswitch interacting with a small gold cluster (Au19+) using time-dependent density functional theory (TD-DFT). The enhancement mechanism (CHEM) due to the moleculesurface chemical coupling in surface-enhanced Raman scattering (SERS) has been characterized for this system. We demonstrate that it is possible to control the CHEM enhancement by switching the photoswitch from its closed form to its open form. The open form of the photoswitch is found to be the strongest Raman scatterer when adsorbed on the surface whereas the opposite is found for the free molecule. This trend is explained using a simple two-state approximation. In this model the CHEM enhancement scales roughly as (X/e)4, where X is the HOMOLUMO gap of the free molecule and e is an average excitation between the HOMO of the photoswitch and the LUMO of the metal. We propose that the ability of this photoswitch to switch reversibly from open to closed will make it an excellent probe to control the CHEM enhancement of SERS.</div></front></TEI><affiliations><list><country><li>États-Unis</li></country><region><li>Pennsylvanie</li></region><settlement><li>University Park (Pennsylvanie)</li></settlement><orgName><li>Université d'État de Pennsylvanie</li></orgName></list><tree><country name="États-Unis"><region name="Pennsylvanie"><name sortKey="Morton, Seth Michael" sort="Morton, Seth Michael" uniqKey="Morton S" first="Seth Michael" last="Morton">Seth Michael Morton</name></region><name sortKey="Ewusi Annan, Ebo" sort="Ewusi Annan, Ebo" uniqKey="Ewusi Annan E" first="Ebo" last="Ewusi-Annan">Ebo Ewusi-Annan</name><name sortKey="Ewusi Annan, Ebo" sort="Ewusi Annan, Ebo" uniqKey="Ewusi Annan E" first="Ebo" last="Ewusi-Annan">Ebo Ewusi-Annan</name><name sortKey="Jensen, Lasse" sort="Jensen, Lasse" uniqKey="Jensen L" first="Lasse" last="Jensen">Lasse Jensen</name><name sortKey="Jensen, Lasse" sort="Jensen, Lasse" uniqKey="Jensen L" first="Lasse" last="Jensen">Lasse Jensen</name><name sortKey="Morton, Seth Michael" sort="Morton, Seth Michael" uniqKey="Morton S" first="Seth Michael" last="Morton">Seth Michael Morton</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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