Visualizing and controlling vibrational wave packets of single molecules

Autores
Brinks, Daan; Stefani, Fernando Daniel; Kulzer, Florian; Hildner, Richard; Taminiau, Tim H.; Avlasevich, Yuri; Müllen, Klaus; Van Hulst, Niek F.
Año de publicación
2010
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The active steering of the pathways taken by chemical reactions and the optimization of energy conversion processes provide striking examples of the coherent control of quantum interference through the use of shaped laser pulses. Experimentally, coherence is usually established by synchronizing a subset of molecules in an ensemble with ultra-short laser pulses. But in complex systems where even chemically identical molecules exist with different conformations and in diverse environments, the synchronized subset will have an intrinsic inhomogeneity that limits the degree of coherent control that can be achieved. A naturaland, indeed, the ultimatesolution to overcoming intrinsic inhomogeneities is the investigation of the behaviour of one molecule at a time. The single-molecule approach has provided useful insights into phenomena as diverse as biomolecular interactions, cellular processes and the dynamics of supercooled liquids and conjugated polymers. Coherent state preparation of single molecules has so far been restricted to cryogenic conditions, whereas at room temperature only incoherent vibrational relaxation pathways have been probed. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a high degree of control, and expect that the approach can be extended to achieve single-molecule coherent control in other complex inhomogeneous systems.
Fil: Brinks, Daan. Institut de Ciencies Fotoniques; España
Fil: Stefani, Fernando Daniel. Institut de Ciencies Fotoniques; España. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Kulzer, Florian. Institut de Ciencies Fotoniques; España
Fil: Hildner, Richard. Institut de Ciencies Fotoniques; España
Fil: Taminiau, Tim H.. Institut de Ciencies Fotoniques; España
Fil: Avlasevich, Yuri. Max Planck Institute for Polymer Research; Alemania
Fil: Müllen, Klaus. Max Planck Institute for Polymer Research; Alemania
Fil: Van Hulst, Niek F.. Institut de Ciencies Fotoniques; España. Institució Catalana de Recerca i Estudis Avancats; España
Materia
Single Molecule
Coherent Control
Laser Control
Ultrafast Spectroscopy
Pulse Shaper
Pulse Shaping
Femtosecond
Fluorescence
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:11336/68887
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/68887
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Visualizing and controlling vibrational wave packets of single moleculesBrinks, DaanStefani, Fernando DanielKulzer, FlorianHildner, RichardTaminiau, Tim H.Avlasevich, YuriMüllen, KlausVan Hulst, Niek F.Single MoleculeCoherent ControlLaser ControlUltrafast SpectroscopyPulse ShaperPulse ShapingFemtosecondFluorescencehttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The active steering of the pathways taken by chemical reactions and the optimization of energy conversion processes provide striking examples of the coherent control of quantum interference through the use of shaped laser pulses. Experimentally, coherence is usually established by synchronizing a subset of molecules in an ensemble with ultra-short laser pulses. But in complex systems where even chemically identical molecules exist with different conformations and in diverse environments, the synchronized subset will have an intrinsic inhomogeneity that limits the degree of coherent control that can be achieved. A naturaland, indeed, the ultimatesolution to overcoming intrinsic inhomogeneities is the investigation of the behaviour of one molecule at a time. The single-molecule approach has provided useful insights into phenomena as diverse as biomolecular interactions, cellular processes and the dynamics of supercooled liquids and conjugated polymers. Coherent state preparation of single molecules has so far been restricted to cryogenic conditions, whereas at room temperature only incoherent vibrational relaxation pathways have been probed. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a high degree of control, and expect that the approach can be extended to achieve single-molecule coherent control in other complex inhomogeneous systems.Fil: Brinks, Daan. Institut de Ciencies Fotoniques; EspañaFil: Stefani, Fernando Daniel. Institut de Ciencies Fotoniques; España. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Kulzer, Florian. Institut de Ciencies Fotoniques; EspañaFil: Hildner, Richard. Institut de Ciencies Fotoniques; EspañaFil: Taminiau, Tim H.. Institut de Ciencies Fotoniques; EspañaFil: Avlasevich, Yuri. Max Planck Institute for Polymer Research; AlemaniaFil: Müllen, Klaus. Max Planck Institute for Polymer Research; AlemaniaFil: Van Hulst, Niek F.. Institut de Ciencies Fotoniques; España. Institució Catalana de Recerca i Estudis Avancats; EspañaNature Publishing Group2010-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/68887Brinks, Daan; Stefani, Fernando Daniel; Kulzer, Florian; Hildner, Richard; Taminiau, Tim H.; et al.; Visualizing and controlling vibrational wave packets of single molecules; Nature Publishing Group; Nature; 465; 7300; 6-2010; 905-9080028-0836CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1038/nature09110info:eu-repo/semantics/altIdentifier/url/https://www.nature.com/articles/nature09110info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:05:55Zoai:ri.conicet.gov.ar:11336/68887instacron: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 10:05:55.355CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Visualizing and controlling vibrational wave packets of single molecules
title Visualizing and controlling vibrational wave packets of single molecules
spellingShingle Visualizing and controlling vibrational wave packets of single molecules
Brinks, Daan
Single Molecule
Coherent Control
Laser Control
Ultrafast Spectroscopy
Pulse Shaper
Pulse Shaping
Femtosecond
Fluorescence
title_short Visualizing and controlling vibrational wave packets of single molecules
title_full Visualizing and controlling vibrational wave packets of single molecules
title_fullStr Visualizing and controlling vibrational wave packets of single molecules
title_full_unstemmed Visualizing and controlling vibrational wave packets of single molecules
title_sort Visualizing and controlling vibrational wave packets of single molecules
dc.creator.none.fl_str_mv Brinks, Daan
Stefani, Fernando Daniel
Kulzer, Florian
Hildner, Richard
Taminiau, Tim H.
Avlasevich, Yuri
Müllen, Klaus
Van Hulst, Niek F.
author Brinks, Daan
author_facet Brinks, Daan
Stefani, Fernando Daniel
Kulzer, Florian
Hildner, Richard
Taminiau, Tim H.
Avlasevich, Yuri
Müllen, Klaus
Van Hulst, Niek F.
author_role author
author2 Stefani, Fernando Daniel
Kulzer, Florian
Hildner, Richard
Taminiau, Tim H.
Avlasevich, Yuri
Müllen, Klaus
Van Hulst, Niek F.
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Single Molecule
Coherent Control
Laser Control
Ultrafast Spectroscopy
Pulse Shaper
Pulse Shaping
Femtosecond
Fluorescence
topic Single Molecule
Coherent Control
Laser Control
Ultrafast Spectroscopy
Pulse Shaper
Pulse Shaping
Femtosecond
Fluorescence
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The active steering of the pathways taken by chemical reactions and the optimization of energy conversion processes provide striking examples of the coherent control of quantum interference through the use of shaped laser pulses. Experimentally, coherence is usually established by synchronizing a subset of molecules in an ensemble with ultra-short laser pulses. But in complex systems where even chemically identical molecules exist with different conformations and in diverse environments, the synchronized subset will have an intrinsic inhomogeneity that limits the degree of coherent control that can be achieved. A naturaland, indeed, the ultimatesolution to overcoming intrinsic inhomogeneities is the investigation of the behaviour of one molecule at a time. The single-molecule approach has provided useful insights into phenomena as diverse as biomolecular interactions, cellular processes and the dynamics of supercooled liquids and conjugated polymers. Coherent state preparation of single molecules has so far been restricted to cryogenic conditions, whereas at room temperature only incoherent vibrational relaxation pathways have been probed. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a high degree of control, and expect that the approach can be extended to achieve single-molecule coherent control in other complex inhomogeneous systems.
Fil: Brinks, Daan. Institut de Ciencies Fotoniques; España
Fil: Stefani, Fernando Daniel. Institut de Ciencies Fotoniques; España. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Kulzer, Florian. Institut de Ciencies Fotoniques; España
Fil: Hildner, Richard. Institut de Ciencies Fotoniques; España
Fil: Taminiau, Tim H.. Institut de Ciencies Fotoniques; España
Fil: Avlasevich, Yuri. Max Planck Institute for Polymer Research; Alemania
Fil: Müllen, Klaus. Max Planck Institute for Polymer Research; Alemania
Fil: Van Hulst, Niek F.. Institut de Ciencies Fotoniques; España. Institució Catalana de Recerca i Estudis Avancats; España
description The active steering of the pathways taken by chemical reactions and the optimization of energy conversion processes provide striking examples of the coherent control of quantum interference through the use of shaped laser pulses. Experimentally, coherence is usually established by synchronizing a subset of molecules in an ensemble with ultra-short laser pulses. But in complex systems where even chemically identical molecules exist with different conformations and in diverse environments, the synchronized subset will have an intrinsic inhomogeneity that limits the degree of coherent control that can be achieved. A naturaland, indeed, the ultimatesolution to overcoming intrinsic inhomogeneities is the investigation of the behaviour of one molecule at a time. The single-molecule approach has provided useful insights into phenomena as diverse as biomolecular interactions, cellular processes and the dynamics of supercooled liquids and conjugated polymers. Coherent state preparation of single molecules has so far been restricted to cryogenic conditions, whereas at room temperature only incoherent vibrational relaxation pathways have been probed. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a high degree of control, and expect that the approach can be extended to achieve single-molecule coherent control in other complex inhomogeneous systems.
publishDate 2010
dc.date.none.fl_str_mv 2010-06
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/11336/68887
Brinks, Daan; Stefani, Fernando Daniel; Kulzer, Florian; Hildner, Richard; Taminiau, Tim H.; et al.; Visualizing and controlling vibrational wave packets of single molecules; Nature Publishing Group; Nature; 465; 7300; 6-2010; 905-908
0028-0836
CONICET Digital
CONICET
url http://hdl.handle.net/11336/68887
identifier_str_mv Brinks, Daan; Stefani, Fernando Daniel; Kulzer, Florian; Hildner, Richard; Taminiau, Tim H.; et al.; Visualizing and controlling vibrational wave packets of single molecules; Nature Publishing Group; Nature; 465; 7300; 6-2010; 905-908
0028-0836
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1038/nature09110
info:eu-repo/semantics/altIdentifier/url/https://www.nature.com/articles/nature09110
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 Nature Publishing Group
publisher.none.fl_str_mv Nature Publishing Group
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 13.070432

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