Efficient singlet exciton fission in pentacene prepared from a soluble precursor

Carrier multiplication using singlet exciton fission (SF) to generate a pair of spin-triplet excitons from a single optical excitation has been highlighted as a promising approach to boost the photocurrent in photovoltaics (PVs) thereby allowing PV operation beyond the Shockley-Queisser limit. The a...

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Published in:APL materials Vol. 4; no. 11; pp. 116112 - 116112-6
Main Authors: Tabachnyk, Maxim, Karani, Arfa H., Broch, Katharina, Pazos-Outón, Luis M., Xiao, James, Jellicoe, Tom C., Novák, Jiří, Harkin, David, Pearson, Andrew J., Rao, Akshay, Greenham, Neil C., Böhm, Marcus L., Friend, Richard H.
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Language:English
Published: AIP Publishing LLC 01-11-2016
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Abstract Carrier multiplication using singlet exciton fission (SF) to generate a pair of spin-triplet excitons from a single optical excitation has been highlighted as a promising approach to boost the photocurrent in photovoltaics (PVs) thereby allowing PV operation beyond the Shockley-Queisser limit. The applicability of many efficient fission materials, however, is limited due to their poor solubility. For instance, while acene-based organics such as pentacene (Pc) show high SF yields (up to200%), the plain acene backbone renders the organic molecule insoluble in common organic solvents. Previous approaches adding solubilizing side groups such as bis(tri-iso-propylsilylethynyl) to the Pc core resulted in low vertical carrier mobilities due to reduction of the transfer integrals via steric hindrance, which prevented high efficiencies in PVs. Here we show how to achieve good solubility while retaining the advantages of molecular Pc by using a soluble precursor route. The precursor fully converts into molecular Pc through thermal removal of the solubilizing side groups upon annealing above 150 °C in the solid state. The annealed precursor shows small differences in the crystallinity compared to evaporated thin films of Pc, indicating that the Pc adopts the bulk rather than surface polytype. Furthermore, we identify identical SF properties such as sub-100 fs fission time and equally long triplet lifetimes in both samples.
AbstractList Carrier multiplication using singlet exciton fission (SF) to generate a pair of spin-triplet excitons from a single optical excitation has been highlighted as a promising approach to boost the photocurrent in photovoltaics (PVs) thereby allowing PV operation beyond the Shockley-Queisser limit. The applicability of many efficient fission materials, however, is limited due to their poor solubility. For instance, while acene-based organics such as pentacene (Pc) show high SF yields (up to200%), the plain acene backbone renders the organic molecule insoluble in common organic solvents. Previous approaches adding solubilizing side groups such as bis(tri-iso-propylsilylethynyl) to the Pc core resulted in low vertical carrier mobilities due to reduction of the transfer integrals via steric hindrance, which prevented high efficiencies in PVs. Here we show how to achieve good solubility while retaining the advantages of molecular Pc by using a soluble precursor route. The precursor fully converts into molecular Pc through thermal removal of the solubilizing side groups upon annealing above 150 °C in the solid state. The annealed precursor shows small differences in the crystallinity compared to evaporated thin films of Pc, indicating that the Pc adopts the bulk rather than surface polytype. Furthermore, we identify identical SF properties such as sub-100 fs fission time and equally long triplet lifetimes in both samples.
Author Tabachnyk, Maxim
Pearson, Andrew J.
Jellicoe, Tom C.
Greenham, Neil C.
Karani, Arfa H.
Xiao, James
Rao, Akshay
Broch, Katharina
Pazos-Outón, Luis M.
Novák, Jiří
Harkin, David
Friend, Richard H.
Böhm, Marcus L.
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Snippet Carrier multiplication using singlet exciton fission (SF) to generate a pair of spin-triplet excitons from a single optical excitation has been highlighted as...
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Title Efficient singlet exciton fission in pentacene prepared from a soluble precursor
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