Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone

Autores
Aruda, Kenneth O.; Bohlmann Kunz, Miriam; Tagliazucchi, Mario Eugenio; Weiss, Emily A.
Año de publicación
2015
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
This paper describes an increase in the yield of collisionally gated photoinduced electron transfer (electron transfer events per collision) from oleate-capped PbS quantum dots (QDs) to benzoquinone (BQ) with increasing temperature (from 0 to 50 °C), due to increased permeability of the oleate adlayer of the QDs to BQ. The same changes in intermolecular structure of the adlayer that increase its permeability to BQ also increase its permeability to the solvent, toluene, resulting in a decrease in viscous drag and an apparent increase in the diffusion coefficient of the QDs, as measured by diffusion-ordered spectroscopy (DOSY) NMR. Comparison of NMR and transient absorption spectra of QDs capped with flexible oleate with those capped with rigid methylthiolate provides evidence that the temperature dependence of the permeability of the oleate ligand shell is due to formation of transient gaps in the adlayer through conformational fluctuations of the ligands.
Fil: Aruda, Kenneth O.. Northwestern University; Estados Unidos
Fil: Bohlmann Kunz, Miriam. Northwestern University; Estados Unidos
Fil: Tagliazucchi, Mario Eugenio. Northwestern University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Weiss, Emily A.. Northwestern University; Estados Unidos
Materia
Pbs
Electron Transfer
Trransient Absortion
Nmr
Quantum Dots
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/80443
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/80443
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinoneAruda, Kenneth O.Bohlmann Kunz, MiriamTagliazucchi, Mario EugenioWeiss, Emily A.PbsElectron TransferTrransient AbsortionNmrQuantum Dotshttps://purl.org/becyt/ford/2.10https://purl.org/becyt/ford/2This paper describes an increase in the yield of collisionally gated photoinduced electron transfer (electron transfer events per collision) from oleate-capped PbS quantum dots (QDs) to benzoquinone (BQ) with increasing temperature (from 0 to 50 °C), due to increased permeability of the oleate adlayer of the QDs to BQ. The same changes in intermolecular structure of the adlayer that increase its permeability to BQ also increase its permeability to the solvent, toluene, resulting in a decrease in viscous drag and an apparent increase in the diffusion coefficient of the QDs, as measured by diffusion-ordered spectroscopy (DOSY) NMR. Comparison of NMR and transient absorption spectra of QDs capped with flexible oleate with those capped with rigid methylthiolate provides evidence that the temperature dependence of the permeability of the oleate ligand shell is due to formation of transient gaps in the adlayer through conformational fluctuations of the ligands.Fil: Aruda, Kenneth O.. Northwestern University; Estados UnidosFil: Bohlmann Kunz, Miriam. Northwestern University; Estados UnidosFil: Tagliazucchi, Mario Eugenio. Northwestern University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Weiss, Emily A.. Northwestern University; Estados UnidosAmerican Chemical Society2015-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/80443Aruda, Kenneth O.; Bohlmann Kunz, Miriam; Tagliazucchi, Mario Eugenio; Weiss, Emily A.; Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone; American Chemical Society; Journal of Physical Chemistry Letters; 6; 14; 7-2015; 2841-28461948-7185CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/acs.jpclett.5b01256info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.5b01256info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:59:03Zoai:ri.conicet.gov.ar:11336/80443instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-10-22 11:59:03.523CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
title Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
spellingShingle Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
Aruda, Kenneth O.
Pbs
Electron Transfer
Trransient Absortion
Nmr
Quantum Dots
title_short Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
title_full Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
title_fullStr Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
title_full_unstemmed Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
title_sort Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone
dc.creator.none.fl_str_mv Aruda, Kenneth O.
Bohlmann Kunz, Miriam
Tagliazucchi, Mario Eugenio
Weiss, Emily A.
author Aruda, Kenneth O.
author_facet Aruda, Kenneth O.
Bohlmann Kunz, Miriam
Tagliazucchi, Mario Eugenio
Weiss, Emily A.
author_role author
author2 Bohlmann Kunz, Miriam
Tagliazucchi, Mario Eugenio
Weiss, Emily A.
author2_role author
author
author
dc.subject.none.fl_str_mv Pbs
Electron Transfer
Trransient Absortion
Nmr
Quantum Dots
topic Pbs
Electron Transfer
Trransient Absortion
Nmr
Quantum Dots
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.10
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv This paper describes an increase in the yield of collisionally gated photoinduced electron transfer (electron transfer events per collision) from oleate-capped PbS quantum dots (QDs) to benzoquinone (BQ) with increasing temperature (from 0 to 50 °C), due to increased permeability of the oleate adlayer of the QDs to BQ. The same changes in intermolecular structure of the adlayer that increase its permeability to BQ also increase its permeability to the solvent, toluene, resulting in a decrease in viscous drag and an apparent increase in the diffusion coefficient of the QDs, as measured by diffusion-ordered spectroscopy (DOSY) NMR. Comparison of NMR and transient absorption spectra of QDs capped with flexible oleate with those capped with rigid methylthiolate provides evidence that the temperature dependence of the permeability of the oleate ligand shell is due to formation of transient gaps in the adlayer through conformational fluctuations of the ligands.
Fil: Aruda, Kenneth O.. Northwestern University; Estados Unidos
Fil: Bohlmann Kunz, Miriam. Northwestern University; Estados Unidos
Fil: Tagliazucchi, Mario Eugenio. Northwestern University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Weiss, Emily A.. Northwestern University; Estados Unidos
description This paper describes an increase in the yield of collisionally gated photoinduced electron transfer (electron transfer events per collision) from oleate-capped PbS quantum dots (QDs) to benzoquinone (BQ) with increasing temperature (from 0 to 50 °C), due to increased permeability of the oleate adlayer of the QDs to BQ. The same changes in intermolecular structure of the adlayer that increase its permeability to BQ also increase its permeability to the solvent, toluene, resulting in a decrease in viscous drag and an apparent increase in the diffusion coefficient of the QDs, as measured by diffusion-ordered spectroscopy (DOSY) NMR. Comparison of NMR and transient absorption spectra of QDs capped with flexible oleate with those capped with rigid methylthiolate provides evidence that the temperature dependence of the permeability of the oleate ligand shell is due to formation of transient gaps in the adlayer through conformational fluctuations of the ligands.
publishDate 2015
dc.date.none.fl_str_mv 2015-07
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/80443
Aruda, Kenneth O.; Bohlmann Kunz, Miriam; Tagliazucchi, Mario Eugenio; Weiss, Emily A.; Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone; American Chemical Society; Journal of Physical Chemistry Letters; 6; 14; 7-2015; 2841-2846
1948-7185
CONICET Digital
CONICET
url http://hdl.handle.net/11336/80443
identifier_str_mv Aruda, Kenneth O.; Bohlmann Kunz, Miriam; Tagliazucchi, Mario Eugenio; Weiss, Emily A.; Temperature-dependent permeability of the ligand shell of pbs quantum dots probed by electron transfer to benzoquinone; American Chemical Society; Journal of Physical Chemistry Letters; 6; 14; 7-2015; 2841-2846
1948-7185
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/acs.jpclett.5b01256
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.5b01256
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 12.982451

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