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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/80443
Ver los metadatos del registro completo
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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 Técnicas2025-09-29T10:26:21Zoai: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:34982025-09-29 10:26:22.022CONICET 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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1844614264930697216 |
score |
13.070432 |