TY - JOUR
T1 - Assessing the nature of the charge-transfer electronic states in organic solar cells
AU - Chen, Xian Kai
AU - Coropceanu, Veaceslav
AU - Brédas, Jean Luc
N1 - Funding Information:
The work was supported by the Department of the Navy, Office of Naval Research, under the MURI “Center for Advanced Organic Photovoltaics” (Awards Nos. N00014-14-1-0580 and N00014-16-1-2520) and under Award No. N00014-17-1-2208, as well as by the National Science Foundation (DMR-1708147). V.C. also acknowledges support by the Institute for Advanced Studies of the Université de Cergy Pontoise under the Paris Seine Initiative for Excellence (“Investissements d’Avenir” ANR-16-IDEX-0008). We acknowledge Dr. Mahesh Kumar Ravva for providing the geometry structures of the PIPCP/PCBM molecular complexes, Dr. Niva A. Ran and Prof. Thuc-Quyen Nguyen for providing the experimental absorption data of the PIPCP/PCBM blend, and Prof. Koen Vandewal for providing the experimental absorption data of the PBTTT/PCBM blend.
Publisher Copyright:
© 2018, The Author(s).
PY - 2018/12/1
Y1 - 2018/12/1
N2 - The charge-transfer electronic states appearing at the donor-acceptor interfaces in organic solar cells mediate exciton dissociation, charge generation, and charge recombination. To date, the characterization of their nature has been carried out on the basis of models that only involve the charge-transfer state and the ground state. Here, we demonstrate that it is essential to go beyond such a two-state model and to consider explicitly as well the electronic and vibrational couplings with the local absorbing state on the donor and/or acceptor. We have thus developed a three-state vibronic model that allows us: to provide a reliable description of the optical absorption features related to the charge-transfer states; to underline the erroneous interpretations stemming from the application of the semi-classical two-state model; and to rationalize how the hybridization between the local-excitation state and charge-transfer state can lead to lower non-radiative voltage losses and higher power conversion efficiencies.
AB - The charge-transfer electronic states appearing at the donor-acceptor interfaces in organic solar cells mediate exciton dissociation, charge generation, and charge recombination. To date, the characterization of their nature has been carried out on the basis of models that only involve the charge-transfer state and the ground state. Here, we demonstrate that it is essential to go beyond such a two-state model and to consider explicitly as well the electronic and vibrational couplings with the local absorbing state on the donor and/or acceptor. We have thus developed a three-state vibronic model that allows us: to provide a reliable description of the optical absorption features related to the charge-transfer states; to underline the erroneous interpretations stemming from the application of the semi-classical two-state model; and to rationalize how the hybridization between the local-excitation state and charge-transfer state can lead to lower non-radiative voltage losses and higher power conversion efficiencies.
UR - http://www.scopus.com/inward/record.url?scp=85058603602&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85058603602&partnerID=8YFLogxK
U2 - 10.1038/s41467-018-07707-8
DO - 10.1038/s41467-018-07707-8
M3 - Article
C2 - 30546009
AN - SCOPUS:85058603602
SN - 2041-1723
VL - 9
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 5295
ER -