Abstract
In this feature article, we discuss the fundamental use of materials-characterization methods that directly determine structural information on the dye···TiO2 interface in dye-sensitized solar cells (DSCs). This interface is usually buried within the DSC and submerged in solvent and electrolyte, which renders such metrological work nontrivial. We will show how ex-situ X-ray reflectometry (XRR), atomic-force microscopy (AFM), grazing-incidence X-ray scattering (GIXS), pair-distribution-function analysis of X-ray diffraction data (gaPDF), and in-situ neutron reflectometry (NR) can be used to deliver specific structural information on the dye···TiO2 interface regarding dye anchoring, dye aggregation, molecular dye orientation, intermolecular spacing between dye molecules, interactions between the dye molecules and the TiO2 surface, and interactions between the dye molecules and the electrolyte components and precursors. Some of these materials-characterization techniques have been developed specifically for this purpose. We will demonstrate how the direct acquisition of such information from materials-characterization experiments is crucial for assembling a holistic structural picture of this interface, which in turn can be used to develop DSC design guidelines. Moreover, we will show how these methodologies can be used in the experimental-validation process of "design-to-device" pipelines for big-data- and machine-learning-based materials discovery. We conclude with an outlook on further developments of this design-to-device approach as well as the materials characterization of more dye···TiO2 interfacial structures that involve known DSC dyes using the methods described herein. In addition, we propose to combine these formally disparate metrologies so that their complementary merits can be exploited simultaneously. New metrologies of this kind could serve as a "one-stop-shop" for the materials characterization of surfaces, interfaces, and bulk structures in DSCs and other devices with layered architectures.