Broadband Ultrafast Photoluminescence Spectroscopy Resolves Charge Photogeneration via De localized Hot Excitons in Polymer:Fullerene Photovoltaic Blends
被引:93
作者:
Chen, Kai
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MacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Victoria Univ Wellington, Sch Chem & Phys Sci, Wellington 6140, New ZealandMacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Chen, Kai
[1
,2
]
Barker, Alex J.
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MacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Victoria Univ Wellington, Sch Chem & Phys Sci, Wellington 6140, New ZealandMacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Barker, Alex J.
[1
,2
]
Reish, Matthew E.
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MacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Univ Otago, Dept Chem, Dunedin 9054, New ZealandMacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Reish, Matthew E.
[1
,3
]
Gordon, Keith C.
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MacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Univ Otago, Dept Chem, Dunedin 9054, New ZealandMacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Gordon, Keith C.
[1
,3
]
Hodgkiss, Justin M.
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MacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Victoria Univ Wellington, Sch Chem & Phys Sci, Wellington 6140, New ZealandMacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
Hodgkiss, Justin M.
[1
,2
]
机构:
[1] MacDiarmid Inst Adv Mat & Nanotechnol, Auckland, New Zealand
[2] Victoria Univ Wellington, Sch Chem & Phys Sci, Wellington 6140, New Zealand
[3] Univ Otago, Dept Chem, Dunedin 9054, New Zealand
Conventional descriptions of excitons in semiconducting polymers do not account for several important observations in polymer:fullerene photovoltaic blends, including the ultrafast time scale of charge photogeneration in phase separated blends and the intermediate role of delocalized charge transfer states. We investigate the nature of excitons in thin films of polymers and polymer:fullerene blends by using broadband ultrafast photoluminescence spectroscopy. Our technique enables us to resolve energetic relaxation, as well as the volume of excitons and population dynamics on ultrafast time scales. We resolve substantial high-energy emission from hot excitons prior to energetic relaxation, which occurs predominantly on a subpicosecond time scale. Consistent with quantum chemical calculations, ultrafast annihilation measurements show that excitons initially extend along a substantial chain length prior to localization induced by structural relaxation. Moreover, we see that hot excitons are initially highly mobile and the subsequent rapid decay in mobility is correlated with energetic relaxation. The relevance of these measurements to charge photogeneration is confirmed by our measurements in blends. We find that charge photogeneration occurs predominately via these delocalized hot exciton states in competition with relaxation and independently of temperature. As well as accounting for the ultrafast time scale of charge generation across large polymer phases, delocalized hot excitons may also account for the crucial requirement that primary charge pairs are well separated in efficient organic photovoltaic blends.
机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA
Univ Mons, Lab Chem Novel Mat, B-7000 Mons, BelgiumGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Bredas, Jean-Luc
;
Norton, Joseph E.
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Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USAGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Norton, Joseph E.
;
Cornil, Jerome
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h-index: 0
机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA
Univ Mons, Lab Chem Novel Mat, B-7000 Mons, BelgiumGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Cornil, Jerome
;
Coropceanu, Veaceslav
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机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USAGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
机构:
Univ Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USA
Dogariu, A
;
Vacar, D
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Univ Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USA
Vacar, D
;
Heeger, AJ
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Univ Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USA
机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA
Univ Mons, Lab Chem Novel Mat, B-7000 Mons, BelgiumGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Bredas, Jean-Luc
;
Norton, Joseph E.
论文数: 0引用数: 0
h-index: 0
机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USAGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Norton, Joseph E.
;
Cornil, Jerome
论文数: 0引用数: 0
h-index: 0
机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA
Univ Mons, Lab Chem Novel Mat, B-7000 Mons, BelgiumGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Cornil, Jerome
;
Coropceanu, Veaceslav
论文数: 0引用数: 0
h-index: 0
机构:
Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USAGeorgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA
机构:
Univ Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USA
Dogariu, A
;
Vacar, D
论文数: 0引用数: 0
h-index: 0
机构:
Univ Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USA
Vacar, D
;
Heeger, AJ
论文数: 0引用数: 0
h-index: 0
机构:
Univ Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USAUniv Calif Santa Barbara, Inst Polymers & Organ Solids, Santa Barbara, CA 93106 USA