This chapter presents the fate of the charge carriers from the moment of its photogeneration in the perovskite to injection and transport into electrodes. Time-resolved electrical measurement techniques, terahertz (THz) spectroscopy and microwave (MW) conductivity, are primarily used to deconvolute ultrafast processes and to directly access behavior of charged species from the ps to µs timescales. Transient absorption and photoluminescence spectroscopy were also utilized to gain insight on carrier population dynamics and radiatively recombining charges. Photogenerated charged species were converted into highly mobile charges (µe = 12.5 cm2V-1s-1 and µh = 7.5 cm2V-1s-1) almost instantaneously (< 0.2 ps), while the remaining loosely bounded excitons dissociate into mobile charges after 2-3 ps. This high mobility is maintained for at least 1 ns as obtained by THz spectroscopy, while its lifetime is at least few tens of µs as measured by the MW conductivity technique. Lowering the temperature increases carrier mobilities with T-1.6.Dependence and a 75 meV barrier energy is required for temperature-activated recombination. Finally, injection of hole from MAPbI3 to Spiro-OMeTAD was found to be ultrafast and the state and population of dark holes dictate its recombination.
Part of the book: Perovskite Materials
The early time charge carrier dynamics in quantum dot‐sensitized and organo‐metal halide perovskite solar cells are presented in this chapter. Using transient spectroscopy techniques, i.e., absorption, photoluminescence, and photoconductivity, we probed the generation mechanism, charge injection, mobility, and recombination of charges in the time scales of subpicosecond (ps) to a nanosecond. In few ps, electron injection from quantum dot to n‐type metal oxide (MO) is complete while hole injection to p‐type MO required hundreds of ps. The injection process is dictated by the band alignment, density of states of MO and the charge transfer state at the interface. For organo‐metal halide perovskite material, there is a distribution of exciton binding energy brought about by the nonuniformity in the quality of the sample. As a result, varying amount of exciton and highly mobile charges may be generated depending on the morphology of the film. In the sample presented here, we found that 30% of photo‐generated charges are excitons, which then dissociates within 2–3 ps. The rest of the photons are instantaneously converted into highly mobile charges (µe = 12.5 cm2 V-1 s-1 and µh = 7.5 cm2 V-1 s-1), and at the appropriate excitation fluence, the photoconductivity remains constant up to 1 ns. The time scale and mechanism of charge injection from perovskite into organic electrodes are also presented.
Part of the book: Nanostructured Solar Cells