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2.
Adv Mater ; 26(16): 2533-9, 2014 Apr 23.
Article in English | MEDLINE | ID: mdl-24574091

ABSTRACT

The field dependence and yield of free charge carrier generation in polymer:fullerene blends with varying energetic offsets is not affected when the excitation energy is varied from above band-gap to direct CT state excitation. Instead, the ability of the CT state to split is dictated by the energetic offset between the relaxed CT state and the charge separated (CS) state.

3.
Nat Mater ; 13(1): 63-8, 2014 Jan.
Article in English | MEDLINE | ID: mdl-24240240

ABSTRACT

Interfaces between organic electron-donating (D) and electron-accepting (A) materials have the ability to generate charge carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold via weakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer:fullerene, small-molecule:C60 and polymer:polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90% without the need for excess electronic or vibrational energy.

4.
J Am Chem Soc ; 135(12): 4656-9, 2013 Mar 27.
Article in English | MEDLINE | ID: mdl-23473262

ABSTRACT

While varying the size and branching of solubilizing side chains in π-conjugated polymers impacts their self-assembling properties in thin-film devices, these structural changes remain difficult to anticipate. This report emphasizes the determining role that linear side-chain substituents play in poly(benzo[1,2-b:4,5-b']dithiophene-thieno[3,4-c]pyrrole-4,6-dione) (PBDTTPD) polymers for bulk heterojunction (BHJ) solar cell applications. We show that replacing branched side chains by linear ones in the BDT motifs induces a critical change in polymer self-assembly and backbone orientation in thin films that correlates with a dramatic drop in solar cell efficiency. In contrast, we show that for polymers with branched alkyl-substituted BDT motifs, controlling the number of aliphatic carbons in the linear N-alkyl-substituted TPD motifs is a major contributor to improved material performance. With this approach, PBDTTPD polymers were found to reach power conversion efficiencies of 8.5% and open-circuit voltages of 0.97 V in BHJ devices with PC71BM, making PBDTTPD one of the best polymer donors for use in the high-band-gap cell of tandem solar cells.

5.
Adv Mater ; 23(45): 5359-63, 2011 Dec 01.
Article in English | MEDLINE | ID: mdl-22021084

ABSTRACT

Efficient organic photovoltaic (OPV) materials are constructed by attaching completely planar, symmetric end-groups to donor-acceptor electroactive small molecules. Appending C2-pyrene as the small molecule end-group to a diketopyrrolopyrrole core leads to materials with a tight, aligned crystal packing and favorable morphology dictated by π-π interactions, resulting in high power conversion efficiencies and high fill factors. The use of end-groups to direct molecular self-assembly is an effective strategy for designing high-performance small molecule OPV devices.


Subject(s)
Electric Power Supplies , Pyrenes/chemistry , Sunlight , Crystallography, X-Ray
7.
J Am Chem Soc ; 132(22): 7595-7, 2010 Jun 09.
Article in English | MEDLINE | ID: mdl-20469863

ABSTRACT

The correlation between the nature of alkyl substituents on N-alkylthieno[3,4-c]pyrrole-4,6-dione (TPD)-based polymers and solar cell device performance has been investigated. After adjusting device parameters, these TPD-based polymers used with PC(61)BM provided photovoltaic responses ranging from 4.0% to 6.8%, depending on the size and shape of the alkyl solubilizing groups. Further, we have correlated the effect of the alkyl groups on the structural order and orientation of the polymer backbone using grazing incidence X-ray scattering analysis, and we have demonstrated how fine-tuning of these parameters can improve the power conversion efficiency.

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