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Non-invasive imaging of the atomic arrangement in two-dimensional (2D)Ruddlesden-Popper hybrid Perovskites (RPPs), as well as understanding therelated effects is challenging, due to the insulating nature and softness ofthe organic layers which also obscure the underlying inorganic lattice. Here,we demonstrate a sub-angstrom resolution imaging of both soft organic layersand inorganic framework in a prototypical 2D lead-halide RPP crystal viacombined tip-functionalized Scanning Tunneling Microscopy (STM) and non-contactAtomic Force Microscope (ncAFM) corroborated by theoretical simulations. STMmeasurements unveil the atomic reconstruction of the inorganic lead-halidelattice and overall twin-domain composition of the RPP crystal, while ncAFMmeasurements with a CO-tip enable non-perturbative visualization of thecooperative reordering of surface organic cations driven by their hydrogenbonding interactions with the inorganic lattice. Moreover, such a jointtechnique also allows for the atomic-scale imaging of the electrostaticpotential variation across the twin-domain walls, revealing alternatingquasi-one-dimensional (1D) electron and hole-channels at neighboringtwin-boundaries, which may influence in-plane exciton transport anddissociation.

Sub-angstrom Non-invasive Imaging of Atomic Arrangement in 2D Hybrid Perovskites