Surface trap states in copper indium gallium
selenide semiconductor nanocrystals (NCs), which serve as undesirable
channels for nonradiative carrier recombination, remain a great challenge
impeding the development of solar and optoelectronics devices based
on these NCs. In order to design efficient passivation techniques
to minimize these trap states, a precise knowledge about the charge
carrier dynamics on the NCs surface is essential. However, selective
mapping of surface traps requires capabilities beyond the reach of
conventional laser spectroscopy and static electron microscopy; it
can only be accessed by using a one-of-a-kind, second-generation four-dimensional
scanning ultrafast electron microscope (4D S-UEM) with subpicosecond
temporal and nanometer spatial resolutions. Here, we precisely map
the collective surface charge carrier dynamics of copper indium gallium
selenide NCs as a function of the surface trap states before and after
surface passivation in real space and time using S-UEM. The time-resolved
snapshots clearly demonstrate that the density of the trap states
is significantly reduced after zinc sulfide (ZnS) shelling. Furthermore,
the removal of trap states and elongation of carrier lifetime are
confirmed by the increased photocurrent of the self-biased photodetector
fabricated using the shelled NCs.