Abstract
A power conversion efficiency of 3.4% with an open-circuit voltage of $1\phantom{\rule{0.3em}{0ex}}\mathrm{V}$ was recently demonstrated in a thin film solar cell utilizing fullerene ${\mathrm{C}}_{60}$ as acceptor and a new acceptor-substituted oligothiophene with an optical gap of $1.77\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$ as donor [K. Schulze et al., Adv. Mater. (Weinheim, Ger.) 18, 2872 (2006)]. This prompted us to systematically study the energy- and electron transfer processes at the oligothiophene:fullerene heterojunction for a homologous series of these oligothiophenes. Cyclic voltammetry and ultraviolet photoelectron spectroscopy data show that the heterojunction is modified due to tuning of the highest occupied molecular orbital energy for different oligothiophene chain lengths, while the lowest unoccupied molecular orbital energy remains essentially fixed due to the presence of electron-withdrawing end groups (dicyanovinyl) attached to the oligothiophene. Use of photoinduced absorption (PA) allows the study of the electron transfer process at the heterojunction to ${\mathrm{C}}_{60}$. Quantum-chemical calculations performed at the density functional theory and/or time-dependent density functional theory level and cation absorption spectra of diluted $\mathrm{DCV}n\mathrm{T}$ provide an unambiguous identification of the transitions observed in the PA spectra. Upon increasing the effective energy gap of the donor-acceptor pair by increasing the ionization energy of the donor, photoinduced electron transfer is eventually replaced with energy transfer, which alters the photovoltaic operation conditions. The optimum open-circuit voltage of a solar cell is thus a trade-off between efficient charge separation at the interface and maximized effective gap. It appears that the open-circuit voltages of $1.0--1.1\phantom{\rule{0.3em}{0ex}}\mathrm{V}$ in our solar cell devices have reached an optimum since higher voltages result in a loss in charge separation efficiency.
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