Generalised Framework for Controlling and Understanding Ion Dynamics with Passivated Lead Halide Perovskites

Metal halide perovskite solar cells have gained widespread attention due to their high efficiency and high defect tolerance. The absorbing perovskite layer is as a mixed electron-ion conductor that supports high rates of ion and charge transport at room temperature, but the migration of mobile defects can lead to degradation pathways. We combine experimental observations and drift-diffusion modelling to demonstrate a new framework to interpret surface photovoltage (SPV) measurements in perovskite systems and mixed electronic ionic conductors more generally. We conclude that the SPV in mixed electronic ionic conductors can be understood in terms of the change in electric potential at the surface associated with changes in the net charge within the semiconductor system. We show that by modifying the interfaces of perovskite bilayers, we may control defect migration behaviour throughout the perovskite bulk. Our new framework for SPV has broad implications for developing strategies to improve the stability of perovskite devices by controlling defect accumulation at interfaces. More generally, in mixed electronic conductors our framework provides new insights into the behaviour of mobile defects and their interaction with photoinduced charges, which are foundational to physical mechanisms in memristivity, logic, impedance, sensors and energy storage

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Dual Mode Kelvin Probe: Featuring Ambient Pressure Photoemission Spectroscopy and Contact Potential Difference

AbstractWe describe a novel dual-mode Kelvin probe featuring ambient pressure Photoemission Spectroscopy (PES), which yields information on the absolute work function (Φ) of a metal and the Ionisation Potential (IP) of a semiconductor, coupled with a high resolution Contact Potential Difference capability which can be extended to Surface Photovoltage measurements. The relative energy resolution are 50 meV for PES and 1-3 meV for CPD. To surmount the limitation of electron scattering in air the incident photon energy is rastered rather than applying a variable retarding electric field as is used UPS. We propose a mechanism of atmospheric ion generation and show that for the metal photoresponse obeys Fowler Theory. The relationship between CPD and photoelectric threshold is a useful tool in characterizing the electrical behavior of materials. We illustrate this with native oxide covered Cu and n-type Si. Further we show that the photoresponse can be used to generate the near Fermi-level Density of States (DOS) in Iron and Nickel-Phthalocyanine