Extending the Light-Harvesting Properties of Transition-Metal Dendrimers
Larsen, Jane LU ; Puntoriero, Fausto ; Pascher, Torbjörn LU ; McClenaghan, Nathan ; Campagna, Sebastiano ; Åkesson, Eva LU
and Sundström, Villy
LU
(2007)
In ChemPhysChem
8(18).
p.2643-2651
- Abstract
- We report a study of the electronic energy-transfer dynamics within the transition-metal polypyridine complex OsRu3pyr6 (Os[(dpp)Ru(bpy{pyrene})2]38+, where dpp=2,3-bis(2-pyridyl)pyrazine and bpy=2,2-bipyridine) after excitation with UV light. By using a broadband visible femtosecond probe, we are able to simultaneously detect both the energy transfer from the peripheral aromatic ligands to the Os center and the sub-picosecond energy transfer from the initially excited Ru-bpy ligand-centered state to the Os triplet metal-to-ligand charge-transfer (MLCT) state. Pyrene energy transfer occurs from both the nonrelaxed and the relaxed S1 states on timescales of 6 and 45 ps, respectively. In both cases, the energy transfer is described by means... (More)
- We report a study of the electronic energy-transfer dynamics within the transition-metal polypyridine complex OsRu3pyr6 (Os[(dpp)Ru(bpy{pyrene})2]38+, where dpp=2,3-bis(2-pyridyl)pyrazine and bpy=2,2-bipyridine) after excitation with UV light. By using a broadband visible femtosecond probe, we are able to simultaneously detect both the energy transfer from the peripheral aromatic ligands to the Os center and the sub-picosecond energy transfer from the initially excited Ru-bpy ligand-centered state to the Os triplet metal-to-ligand charge-transfer (MLCT) state. Pyrene energy transfer occurs from both the nonrelaxed and the relaxed S1 states on timescales of 6 and 45 ps, respectively. In both cases, the energy transfer is described by means of Förster energy transfer theory. Sub-picosecond energy transfer within the OsRu3 metal-ligand core most likely includes a direct energy transfer between the higher-lying ligand-centered states on Ru and Os, in addition to the transfer between the MLCT states. The absorption cross-sections in both the UV and the visible spectral regions are enhanced by attaching the aromatic pyrene ligands. Furthermore, energy transfer is directed only towards the Os core, which ultimately leads to an exclusive population of the Os-based triplet MLCT state, thus making the OsRu3pyr6 transition metal-polypyridine dendrimer an obvious candidate for artificial light-harvesting systems. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/954006
- author
- Larsen, Jane
LU
; Puntoriero, Fausto
; Pascher, Torbjörn
LU
; McClenaghan, Nathan
; Campagna, Sebastiano
; Åkesson, Eva
LU
and Sundström, Villy
LU
- organization
- publishing date
- 2007
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- dendrimers • excitation energy transfer • light-harvesting systems • time-resolved spectroscopy • transition metals
- in
- ChemPhysChem
- volume
- 8
- issue
- 18
- pages
- 2643 - 2651
- publisher
- John Wiley & Sons Inc.
- external identifiers
-
- wos:000252503700011
- scopus:38049005852
- ISSN
- 1439-7641
- DOI
- 10.1002/cphc.200700539
- language
- English
- LU publication?
- yes
- additional info
- The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
- id
- cbb9c5a5-97b4-48a6-8692-507a42120155 (old id 954006)
- date added to LUP
- 2016-04-01 12:30:52
- date last changed
- 2023-04-05 15:03:45
@article{cbb9c5a5-97b4-48a6-8692-507a42120155,
abstract = {{We report a study of the electronic energy-transfer dynamics within the transition-metal polypyridine complex OsRu3pyr6 (Os[(dpp)Ru(bpy{pyrene})2]38+, where dpp=2,3-bis(2-pyridyl)pyrazine and bpy=2,2-bipyridine) after excitation with UV light. By using a broadband visible femtosecond probe, we are able to simultaneously detect both the energy transfer from the peripheral aromatic ligands to the Os center and the sub-picosecond energy transfer from the initially excited Ru-bpy ligand-centered state to the Os triplet metal-to-ligand charge-transfer (MLCT) state. Pyrene energy transfer occurs from both the nonrelaxed and the relaxed S1 states on timescales of 6 and 45 ps, respectively. In both cases, the energy transfer is described by means of Förster energy transfer theory. Sub-picosecond energy transfer within the OsRu3 metal-ligand core most likely includes a direct energy transfer between the higher-lying ligand-centered states on Ru and Os, in addition to the transfer between the MLCT states. The absorption cross-sections in both the UV and the visible spectral regions are enhanced by attaching the aromatic pyrene ligands. Furthermore, energy transfer is directed only towards the Os core, which ultimately leads to an exclusive population of the Os-based triplet MLCT state, thus making the OsRu3pyr6 transition metal-polypyridine dendrimer an obvious candidate for artificial light-harvesting systems.}},
author = {{Larsen, Jane and Puntoriero, Fausto and Pascher, Torbjörn and McClenaghan, Nathan and Campagna, Sebastiano and Åkesson, Eva and Sundström, Villy}},
issn = {{1439-7641}},
keywords = {{dendrimers • excitation energy transfer • light-harvesting systems • time-resolved spectroscopy • transition metals}},
language = {{eng}},
number = {{18}},
pages = {{2643--2651}},
publisher = {{John Wiley & Sons Inc.}},
series = {{ChemPhysChem}},
title = {{Extending the Light-Harvesting Properties of Transition-Metal Dendrimers}},
url = {{http://dx.doi.org/10.1002/cphc.200700539}},
doi = {{10.1002/cphc.200700539}},
volume = {{8}},
year = {{2007}},
}