Nonthermalized Electron Transport in Dye-Sensitized Nanocrystalline TiO2 Films: Transient Photocurrent and Random-Walk Modeling Studies

Abstract

A random-walk approach is developed to model the electron-transport dynamics in dye-sensitized TiO2 solar cells within a multiple-trapping framework, and the predicted results are compared with those measured by transient photocurrent. The illumination geometry and the wavelength of the probe light are used to create certain initial spatial distributions of photoinjected electrons in the TiO2 films. Both have a dramatic effect on the shape of the measured photocurrent transient. Cells are probed with light incident from either the collecting (substrate) electrode side or the counter-electrode side. Excellent correspondence between simulated and measured current transients is observed. When electrons are injected far from the collecting electrode, their diffusion is found to be classical, corresponding to thermalized (nondispersive) transport. Nonthermalized (dispersive) electron transport is shown to be important when electrons are injected near the collecting electrode, which corresponds to the illuminat...