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Positron annihilationlifetime spectroscopy and positron-electron momentum density (PEMD) studies on multilayers ofPbSe nanocrystals (NCs),supported by transmission electronmicroscopy, show that positrons are strongly trapped at NC surfaces, where they provide insight into thesurface composition andelectronic structure of PbSeNCs. Our analysis indicates abundant annihilation of positrons with Se electrons at the NC surfaces and with O electronsof the oleic ligands bound to Pb ad-atoms at the NC surfaces, which demonstrates that positrons can be used as a sensitive probeto investigate the surface physics and chemistry of nanocrystals inside multilayers. electronicstructure calculations provide detailed insight in the valence and semi-core electron contributionsto the positron-electron momentum density of PbSe. Both lifetime and PEMD are found to correlate with changes in the particlemorphology characteristic of partial ligand removal.


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