Direct observation of ultrafast long-range charge separation at polymer–fullerene heterojunctions
In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer...
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| Published in: | Nature communications Vol. 5; no. 1; p. 4288 |
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| Main Authors: | , , , , , , , , , |
| Format: | Journal Article |
| Language: | English |
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01.07.2014
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| ISSN: | 2041-1723, 2041-1723 |
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| Abstract | In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on ≲50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials.
Photocarrier generation at organic semiconductor heterojunctions is a crucial process, yet its mechanism and dynamics remain unclear. Here, Provencher
et al.
show little change in polymer structure following the charge-transfer process and interpret the observation in terms of unbounded electron-hole pairs. |
|---|---|
| AbstractList | In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on [<, ~]50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials. In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on ≲ 50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials. In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on ≲ 50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials.In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on ≲ 50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials. In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on ≲50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials. Photocarrier generation at organic semiconductor heterojunctions is a crucial process, yet its mechanism and dynamics remain unclear. Here, Provencher et al. show little change in polymer structure following the charge-transfer process and interpret the observation in terms of unbounded electron-hole pairs. |
| ArticleNumber | 4288 |
| Author | Stingelin, Natalie Silva, Carlos Provencher, Françoise Hellmann, Christoph Parker, Anthony W. Bérubé, Nicolas Towrie, Michael Greetham, Gregory M. Côté, Michel Hayes, Sophia C. |
| Author_xml | – sequence: 1 givenname: Françoise surname: Provencher fullname: Provencher, Françoise organization: Département de Physique and Regroupement Québécois sur les Matériaux de Pointe, Université de Montréal, C.P. 6128, Succursale Centre-Ville – sequence: 2 givenname: Nicolas surname: Bérubé fullname: Bérubé, Nicolas organization: Département de Physique and Regroupement Québécois sur les Matériaux de Pointe, Université de Montréal, C.P. 6128, Succursale Centre-Ville – sequence: 3 givenname: Anthony W. surname: Parker fullname: Parker, Anthony W. organization: Central Laser Facility, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Oxford – sequence: 4 givenname: Gregory M. surname: Greetham fullname: Greetham, Gregory M. organization: Central Laser Facility, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Oxford – sequence: 5 givenname: Michael surname: Towrie fullname: Towrie, Michael organization: Central Laser Facility, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Oxford – sequence: 6 givenname: Christoph surname: Hellmann fullname: Hellmann, Christoph organization: Department of Materials, Centre for Plastic Electronics, Imperial College London, South Kensington Campus – sequence: 7 givenname: Michel surname: Côté fullname: Côté, Michel organization: Département de Physique and Regroupement Québécois sur les Matériaux de Pointe, Université de Montréal, C.P. 6128, Succursale Centre-Ville – sequence: 8 givenname: Natalie surname: Stingelin fullname: Stingelin, Natalie organization: Department of Materials, Centre for Plastic Electronics, Imperial College London, South Kensington Campus – sequence: 9 givenname: Carlos surname: Silva fullname: Silva, Carlos email: carlos.silva@umontreal.ca organization: Département de Physique and Regroupement Québécois sur les Matériaux de Pointe, Université de Montréal, C.P. 6128, Succursale Centre-Ville, Department of Physics, Imperial College London, South Kensington Campus – sequence: 10 givenname: Sophia C. surname: Hayes fullname: Hayes, Sophia C. email: shayes@ucy.ac.cy organization: Department of Chemistry, University of Cyprus, P.O. Box 20537 |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/24980429$$D View this record in MEDLINE/PubMed |
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| Title | Direct observation of ultrafast long-range charge separation at polymer–fullerene heterojunctions |
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