Kinetic Simulations Of Charge Injection Kinetics From Ultrafast Experiments To Steady State Conditions

We are building towards a multiscale description of solar energy conversion in dye-sensitized solar cells (DSSC). We reported in an initial study a kinetic framework for the femtosecond to microsecond photophysics of a set of ruthenium complexes in solution that produces simulated time-resolved spectroscopic signals that are in quantitative agreement with experiments. Additionally, we have demonstrated that datasets of dynamical observations and steady state measurements are both necessary to predict dye interactions under 1-sun conditions. We discuss extensions of our kinetic framework to 1) compare the excitation and decay kinetics of ruthenium complexes in solution and on ZrO₂ films where there is no charge transfer, 2) establish competing intramolecular transitions and charge transfer to TiO₂, and 3) illustrate that by including explicit experimental interactions in our model, rate coefficients for charge injection, not phenomenological lifetimes, are estimated. Results for simulations under solar irradiance are discussed in context of DSSCs.