Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
Intramolecular charge transfer (CT) processes play a crucial role in fields such as energy conversion, molecular electronics, and biochemistry. Defined by the movement of electronic charge between donor and acceptor groups within a molecule, CT is inherently coupled with nuclear motions, making it e...
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| Format: | Article |
| Language: | English |
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American Association for the Advancement of Science (AAAS)
2025-01-01
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| Series: | Ultrafast Science |
| Online Access: | https://spj.science.org/doi/10.34133/ultrafastscience.0108 |
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| author | Daniele Mocci Juan Reino González Yingxuan Wu Jesús González Vázquez Federico Vismarra Francisco Fernández-Villoria Javier Urieta-Mora Alicia Palacios Pedro Recio Javier Cachon Luis Bañares Matteo Lucchini Maurizio Reduzzi Rocío Borrego-Varillas Nazario Martín Fernando Martín Mauro Nisoli |
| author_facet | Daniele Mocci Juan Reino González Yingxuan Wu Jesús González Vázquez Federico Vismarra Francisco Fernández-Villoria Javier Urieta-Mora Alicia Palacios Pedro Recio Javier Cachon Luis Bañares Matteo Lucchini Maurizio Reduzzi Rocío Borrego-Varillas Nazario Martín Fernando Martín Mauro Nisoli |
| author_sort | Daniele Mocci |
| collection | DOAJ |
| description | Intramolecular charge transfer (CT) processes play a crucial role in fields such as energy conversion, molecular electronics, and biochemistry. Defined by the movement of electronic charge between donor and acceptor groups within a molecule, CT is inherently coupled with nuclear motions, making it essential for the understanding of energy flow and reaction mechanisms in molecular systems. Here, we employ attosecond pump-probe spectroscopy to explore the ultrafast dynamics of 4-amino-4′-nitrobiphenyl (ANB), a donor–π–acceptor molecule. Our experimental results in combination with time-dependent density functional theory and trajectory surface hopping simulations uncover a complex temporal evolution of CT spanning from a few to tens of femtoseconds. The process unfolds in distinct stages. An initial phase is marked by an ultrafast charge migration driven by a molecular planarization process, and it is followed by oscillations in the charge distribution that have a 2-fold origin: the electronic coherence induced by the broadband attosecond pulse and the coupling with nuclear motion. In ANB, these dynamics are exemplified by oscillations in charge density and structural parameters, such as dihedral angles and bond lengths, underscoring the interconnection between electronic and nuclear degrees of freedom. |
| format | Article |
| id | doaj-art-823c9ef2b0dd4e68ba2f374e0c216b70 |
| institution | DOAJ |
| issn | 2765-8791 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | American Association for the Advancement of Science (AAAS) |
| record_format | Article |
| series | Ultrafast Science |
| spelling | doaj-art-823c9ef2b0dd4e68ba2f374e0c216b702025-08-20T03:02:37ZengAmerican Association for the Advancement of Science (AAAS)Ultrafast Science2765-87912025-01-01510.34133/ultrafastscience.0108Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl MoleculeDaniele Mocci0Juan Reino González1Yingxuan Wu2Jesús González Vázquez3Federico Vismarra4Francisco Fernández-Villoria5Javier Urieta-Mora6Alicia Palacios7Pedro Recio8Javier Cachon9Luis Bañares10Matteo Lucchini11Maurizio Reduzzi12Rocío Borrego-Varillas13Nazario Martín14Fernando Martín15Mauro Nisoli16Department of Physics, Politecnico di Milano, 20133 Milano, Italy.Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanoscience), Cantoblanco, 28049 Madrid, Spain.Department of Physics, Politecnico di Milano, 20133 Milano, Italy.Departamento de Química, Universidad Autónoma de Madrid, Cantoblanco, 28049 Madrid, Spain.Department of Physics, Politecnico di Milano, 20133 Milano, Italy.Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanoscience), Cantoblanco, 28049 Madrid, Spain.Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanoscience), Cantoblanco, 28049 Madrid, Spain.Departamento de Química, Universidad Autónoma de Madrid, Cantoblanco, 28049 Madrid, Spain.Departamento de Química Física, Universidad Complutense de Madrid, 28040 Madrid, Spain.Departamento de Química Física, Universidad Complutense de Madrid, 28040 Madrid, Spain.Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanoscience), Cantoblanco, 28049 Madrid, Spain.Department of Physics, Politecnico di Milano, 20133 Milano, Italy.Department of Physics, Politecnico di Milano, 20133 Milano, Italy.Institute for Photonics and Nanotechnologies, IFN-CNR, 20133 Milano, Italy.Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanoscience), Cantoblanco, 28049 Madrid, Spain.Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanoscience), Cantoblanco, 28049 Madrid, Spain.Department of Physics, Politecnico di Milano, 20133 Milano, Italy.Intramolecular charge transfer (CT) processes play a crucial role in fields such as energy conversion, molecular electronics, and biochemistry. Defined by the movement of electronic charge between donor and acceptor groups within a molecule, CT is inherently coupled with nuclear motions, making it essential for the understanding of energy flow and reaction mechanisms in molecular systems. Here, we employ attosecond pump-probe spectroscopy to explore the ultrafast dynamics of 4-amino-4′-nitrobiphenyl (ANB), a donor–π–acceptor molecule. Our experimental results in combination with time-dependent density functional theory and trajectory surface hopping simulations uncover a complex temporal evolution of CT spanning from a few to tens of femtoseconds. The process unfolds in distinct stages. An initial phase is marked by an ultrafast charge migration driven by a molecular planarization process, and it is followed by oscillations in the charge distribution that have a 2-fold origin: the electronic coherence induced by the broadband attosecond pulse and the coupling with nuclear motion. In ANB, these dynamics are exemplified by oscillations in charge density and structural parameters, such as dihedral angles and bond lengths, underscoring the interconnection between electronic and nuclear degrees of freedom.https://spj.science.org/doi/10.34133/ultrafastscience.0108 |
| spellingShingle | Daniele Mocci Juan Reino González Yingxuan Wu Jesús González Vázquez Federico Vismarra Francisco Fernández-Villoria Javier Urieta-Mora Alicia Palacios Pedro Recio Javier Cachon Luis Bañares Matteo Lucchini Maurizio Reduzzi Rocío Borrego-Varillas Nazario Martín Fernando Martín Mauro Nisoli Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule Ultrafast Science |
| title | Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule |
| title_full | Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule |
| title_fullStr | Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule |
| title_full_unstemmed | Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule |
| title_short | Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule |
| title_sort | ultrafast structural reorganization and charge dynamics in a photoionized donor acceptor biphenyl molecule |
| url | https://spj.science.org/doi/10.34133/ultrafastscience.0108 |
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