Understanding surface potential dynamics of passivated perovskites via Kelvin Probe Force Microscopy

Abstract: Molecular passivation has become central to reducing photovoltage losses in metal-halide perovskite solar cells, but its electronic action is still often inferred from device-level metrics rather than directly resolved at the nanoscale. Here, we use amplitude-modulated Kelvin probe force microscopy to examine how [3-(2-aminoethylamino)propyl]trimethoxysilane (AEAPTMS) modifies the surface potential and photovoltage dynamics of mixed-cation, mixed-halide perovskite thin films. AEAPTMS homogenises the dark contact potential difference (CPD), narrowing its distribution from ~45.7 to ~14.6 mV without obvious morphological changes. Under illumination, passivated films show a larger steady-state surface photovoltage (SPV) and faster stabilisation, with the SPV increasing from ~345 to ~417 mV and the stabilisation time constant decreasing from ~840 to ~470 s. Wavelength-dependent SPV further indicates reduced sub-bandgap electronic disorder. By separating grain-boundary and grain-interior contributions, we show that AEAPTMS suppresses grain-boundary potential barriers, linking amino-silane passivation to a more homogeneous and stable carrier landscape.