Imaging and controlling coherent phonon wave packets in single graphene nanoribbons

The motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. Th...

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Autores: Luo, Yang, Pisarra, Michele, Garg, Manish, Kern, Klaus, Martín Jiménez, Alberto, Martín García, Fernando
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/708678
Acceso en línea:http://hdl.handle.net/10486/708678
https://dx.doi.org/10.1038/s41467-023-39239-1
Access Level:acceso abierto
Palabra clave:Graphene
Raman Spectroscopy
Spectrum
Electric Potential
Phonon
Química
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spelling Imaging and controlling coherent phonon wave packets in single graphene nanoribbonsLuo, YangPisarra, MicheleGarg, ManishKern, KlausMartín Jiménez, AlbertoMartín García, FernandoGrapheneRaman SpectroscopySpectrumElectric PotentialPhononQuímicaThe motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. These coherent dynamics occur on the ultrafast timescale, as revealed, e.g., by nonlocal ultrafast vibrational spectroscopic measurements in bulk molecular ensembles and solids. Tracking and controlling vibrational coherences locally at the atomic and molecular scales is, however, much more challenging and in fact has remained elusive so far. Here, we demonstrate that the vibrational coherences induced by broadband laser pulses on a single graphene nanoribbon (GNR) can be probed by femtosecond coherent anti-Stokes Raman spectroscopy (CARS) when performed in a scanning tunnelling microscope (STM). In addition to determining dephasing (~440 fs) and population decay times (~1.8 ps) of the generated phonon wave packets, we are able to track and control the corresponding quantum coherences, which we show to evolve on time scales as short as ~70 fs. We demonstrate that a two-dimensional frequency correlation spectrum unequivocally reveals the quantum couplings between different phonon modes in the GNRPID2019-105458RB-I00, CEX2020-001039-S, CEX2018-000805-M, Comunidad de Madrid Synergy Grant FULMATENNature ResearchDepartamento de QuímicaFacultad de Ciencias20232023-06-13research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/708678https://dx.doi.org/10.1038/s41467-023-39239-1reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7086782026-06-23T12:46:27Z
dc.title.none.fl_str_mv Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
title Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
spellingShingle Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
Luo, Yang
Graphene
Raman Spectroscopy
Spectrum
Electric Potential
Phonon
Química
title_short Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
title_full Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
title_fullStr Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
title_full_unstemmed Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
title_sort Imaging and controlling coherent phonon wave packets in single graphene nanoribbons
dc.creator.none.fl_str_mv Luo, Yang
Pisarra, Michele
Garg, Manish
Kern, Klaus
Martín Jiménez, Alberto
Martín García, Fernando
author Luo, Yang
author_facet Luo, Yang
Pisarra, Michele
Garg, Manish
Kern, Klaus
Martín Jiménez, Alberto
Martín García, Fernando
author_role author
author2 Pisarra, Michele
Garg, Manish
Kern, Klaus
Martín Jiménez, Alberto
Martín García, Fernando
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv Departamento de Química
Facultad de Ciencias
dc.subject.none.fl_str_mv Graphene
Raman Spectroscopy
Spectrum
Electric Potential
Phonon
Química
topic Graphene
Raman Spectroscopy
Spectrum
Electric Potential
Phonon
Química
description The motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. These coherent dynamics occur on the ultrafast timescale, as revealed, e.g., by nonlocal ultrafast vibrational spectroscopic measurements in bulk molecular ensembles and solids. Tracking and controlling vibrational coherences locally at the atomic and molecular scales is, however, much more challenging and in fact has remained elusive so far. Here, we demonstrate that the vibrational coherences induced by broadband laser pulses on a single graphene nanoribbon (GNR) can be probed by femtosecond coherent anti-Stokes Raman spectroscopy (CARS) when performed in a scanning tunnelling microscope (STM). In addition to determining dephasing (~440 fs) and population decay times (~1.8 ps) of the generated phonon wave packets, we are able to track and control the corresponding quantum coherences, which we show to evolve on time scales as short as ~70 fs. We demonstrate that a two-dimensional frequency correlation spectrum unequivocally reveals the quantum couplings between different phonon modes in the GNR
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-06-13
dc.type.none.fl_str_mv research article
http://purl.org/coar/resource_type/c_2df8fbb1
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10486/708678
https://dx.doi.org/10.1038/s41467-023-39239-1
url http://hdl.handle.net/10486/708678
https://dx.doi.org/10.1038/s41467-023-39239-1
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Nature Research
publisher.none.fl_str_mv Nature Research
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
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