  Nonradiative processes limit optoelectronic functionality of nanocrystals and
curb their device performance. Nevertheless, the dynamic structural origins of
nonradiative relaxations in nanocrystals are not understood. Here, femtosecond
electron diffraction measurements corroborated by atomistic simulations uncover
transient lattice deformations accompanying radiationless electronic processes
in semiconductor nanocrystals. Investigation of the excitation energy
dependence shows that hot carriers created by a photon energy considerably
larger than the bandgap induce structural distortions at nanocrystal surfaces
on few picosecond timescales associated with the localization of trapped holes.
On the other hand, carriers created by a photon energy close to the bandgap
result in transient lattice heating that occurs on a much longer 200 ps
timescale, governed by an Auger heating mechanism. Elucidation of the
structural deformations associated with the surface trapping of hot holes
provides atomic-scale insights into the mechanisms deteriorating optoelectronic
performance and a pathway towards minimizing these losses in nanocrystal
devices.
