Abstract
Understanding the ultrafast dynamics of excited state evolution and carrier generation at the complicated titania/dye/electrolyte interface is crucial for the development of narrow energy-gap organic dyes to enhance the performance of dye-sensitized solar cells (DSCs). We herein modulate the energy-levels of N-annulated perylene dyes in significant measure by use of benzothiadiazole-benzoic acid (BTBA) and pyridothiadiazole-benzoic acid (PTBA) segments as the electron-acceptors. Based on the model of cold vs hot excited states for electron injection in DSCs, we have perceived from femtosecond transient absorption measurements that a driving force diminution does not necessarily cause a deceleration of electron injection from the hot excited state to titania, suggesting a crucial role of electron coupling on interfacial charge transfer kinetics. Moreover, the electron-accetpor variation from BTBA to PTBA brings forth a fast relaxation of the hot excited state as well as a rapid deactivation of the cold exc...
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