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Journal of Spectroscopy
Volume 2017 (2017), Article ID 6867507, 16 pages
Research Article

Ultrafast Charge and Triplet State Formation in Diketopyrrolopyrrole Low Band Gap Polymer/Fullerene Blends: Influence of Nanoscale Morphology of Organic Photovoltaic Materials on Charge Recombination to the Triplet State

1Molecular Photonics Group, Van’t Hoff Institute for Molecular Sciences (HIMS), Universiteit van Amsterdam, Science Park 904, 1098 XH Amsterdam, Netherlands
2Molecular Materials and Nanosystems, Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, Netherlands

Correspondence should be addressed to René M. Williams; ln.avu@smailliw.m.r and René A. J. Janssen; ln.eut@nessnaj.j.a.r

Received 19 October 2016; Accepted 25 December 2016; Published 13 April 2017

Academic Editor: Jau-Wern Chiou

Copyright © 2017 René M. Williams et al. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.


Femtosecond transient absorption spectroscopy of thin films of two types of morphologies of diketopyrrolopyrrole low band gap polymer/fullerene-adduct blends is presented and indicates triplet state formation by charge recombination, an important loss channel in organic photovoltaic materials. At low laser fluence (approaching solar intensity) charge formation characterized by a 1350 nm band (in ~250 fs) dominates in the two PDPP-PCBM blends with different nanoscale morphologies and these charges recombine to form a local polymer-based triplet state on the sub-ns timescale (in ~300 and ~900 ps) indicated by an 1100 nm absorption band. The rate of triplet state formation is influenced by the morphology. The slower rate of charge recombination to the triplet state (in ~900 ps) belongs to a morphology that results in a higher power conversion efficiency in the corresponding device. Nanoscale morphology not only influences interfacial area and conduction of holes and electrons but also influences the mechanism of intersystem crossing (ISC). We present a model that correlates morphology to the exchange integral and fast and slow mechanisms for ISC (SOCT-ISC and H-HFI-ISC). For the pristine polymer, a flat and unstructured singlet-singlet absorption spectrum (between 900 and 1400 nm) and a very minor triplet state formation (5%) are observed at low laser fluence.