Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection
Nonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electro...
| Autores: | , , , , , , , , , |
|---|---|
| Formato: | artículo |
| Fecha de publicación: | 2015 |
| País: | España |
| Recursos: | Universidad Autónoma de Madrid |
| Repositorio: | Biblos-e Archivo. Repositorio Institucional de la UAM |
| Idioma: | inglés |
| OAI Identifier: | oai:repositorio.uam.es:10486/676274 |
| Acesso em linha: | http://hdl.handle.net/10486/676274 https://dx.doi.org/10.1088/1367-2630/17/11/113023 |
| Access Level: | acceso abierto |
| Palavra-chave: | Sub-femtosecond laser control Molecular dynamics Conical intersection Nonadiabatic effects Química |
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Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersectionRichter, MariaBouakline, FoudhilGonzález Vázquez, JesúsMartínez-Fernández, LaraCorral Pérez, InésPatchkovskii, SergueiMorales, FelipeIvanov, MishaMartín García, FernandoSmirnova, OlgaSub-femtosecond laser controlMolecular dynamicsConical intersectionNonadiabatic effectsQuímicaNonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electron-nuclear dynamics at CIs, offered by the advent of nearly single-cycle, phase-stable, mid-infrared laser pulses. To illustrate the control mechanism, a two-dimensional model of the NO2 molecule is considered. The key idea of the control scheme is to match the time scale of the laser field oscillations to the characteristic time scale of the wave packet transit through the CI. The instantaneous laser field changes the shape and position of the CI as the wave packet passes through. As the CI moves in the laser field, it 'slices' through the wave packet, sculpting it in the coordinate and momentum space in a way that is sensitive to the carrier-envelope phase of the control pulse. We find that the electronic coherence imparted on the sub-laser-cycle time scale manifests during much longer nuclear dynamics that follow on the many tens of femtosecond time scale. Control efficiency as a function of molecular orientation is analyzed, showing that modest alignment is sufficient for showing the described effectsThis work has been financially supported by the ERA-Chemistry Project PIM2010EEC-00751, DFG SM 292/3-1, the EU FP7 Marie Curie ITN CORINF, the EPSRC Programme Grant No. EP/I032517/1, the European Research Council Advanced Grant No. XCHEM 290853, the MINECO projects FIS2013-42002-R and CTQ2012-35513-C02, a MINECO FPU grant (LMF), the European COST Action XLIC CM1204, and the CAM project NANOFRONTMAG, which are gratefully acknowledged. We also acknowledge allocation of computer time from Mare Nostrum BSC and CCC-UAMInstitute of Physics PublishingDepartamento de QuímicaFacultad de Ciencias20152015-11-06research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/676274https://dx.doi.org/10.1088/1367-2630/17/11/113023reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengEuropean Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 264951European Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 290853open accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/6762742026-06-23T12:46:27Z |
| dc.title.none.fl_str_mv |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| title |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| spellingShingle |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection Richter, Maria Sub-femtosecond laser control Molecular dynamics Conical intersection Nonadiabatic effects Química |
| title_short |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| title_full |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| title_fullStr |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| title_full_unstemmed |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| title_sort |
Sub-laser-cycle control of coupled electron-nuclear dynamics at a conical intersection |
| dc.creator.none.fl_str_mv |
Richter, Maria Bouakline, Foudhil González Vázquez, Jesús Martínez-Fernández, Lara Corral Pérez, Inés Patchkovskii, Serguei Morales, Felipe Ivanov, Misha Martín García, Fernando Smirnova, Olga |
| author |
Richter, Maria |
| author_facet |
Richter, Maria Bouakline, Foudhil González Vázquez, Jesús Martínez-Fernández, Lara Corral Pérez, Inés Patchkovskii, Serguei Morales, Felipe Ivanov, Misha Martín García, Fernando Smirnova, Olga |
| author_role |
author |
| author2 |
Bouakline, Foudhil González Vázquez, Jesús Martínez-Fernández, Lara Corral Pérez, Inés Patchkovskii, Serguei Morales, Felipe Ivanov, Misha Martín García, Fernando Smirnova, Olga |
| author2_role |
author author author author author author author author author |
| dc.contributor.none.fl_str_mv |
Departamento de Química Facultad de Ciencias |
| dc.subject.none.fl_str_mv |
Sub-femtosecond laser control Molecular dynamics Conical intersection Nonadiabatic effects Química |
| topic |
Sub-femtosecond laser control Molecular dynamics Conical intersection Nonadiabatic effects Química |
| description |
Nonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electron-nuclear dynamics at CIs, offered by the advent of nearly single-cycle, phase-stable, mid-infrared laser pulses. To illustrate the control mechanism, a two-dimensional model of the NO2 molecule is considered. The key idea of the control scheme is to match the time scale of the laser field oscillations to the characteristic time scale of the wave packet transit through the CI. The instantaneous laser field changes the shape and position of the CI as the wave packet passes through. As the CI moves in the laser field, it 'slices' through the wave packet, sculpting it in the coordinate and momentum space in a way that is sensitive to the carrier-envelope phase of the control pulse. We find that the electronic coherence imparted on the sub-laser-cycle time scale manifests during much longer nuclear dynamics that follow on the many tens of femtosecond time scale. Control efficiency as a function of molecular orientation is analyzed, showing that modest alignment is sufficient for showing the described effects |
| publishDate |
2015 |
| dc.date.none.fl_str_mv |
2015 2015-11-06 |
| 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/10486/676274 https://dx.doi.org/10.1088/1367-2630/17/11/113023 |
| url |
http://hdl.handle.net/10486/676274 https://dx.doi.org/10.1088/1367-2630/17/11/113023 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.relation.none.fl_str_mv |
European Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 264951 European Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 290853 |
| 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 |
Institute of Physics Publishing |
| publisher.none.fl_str_mv |
Institute of Physics Publishing |
| 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 |
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Biblos-e Archivo. Repositorio Institucional de la UAM |
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1869416755940556800 |
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15.301603 |