[en] Within semiconductor quantum dots (QDs), exciton recombination processes are noteworthy
for depending on the nature of surface coordination and nanocrystal/ligand bonding.
The influence of the molecular surroundings on QDs optoelectronic properties is therefore
intensively studied. Here, from the converse point of view, we anlayze and model the
influence of QDs optoelectronic properties on their ligands. As revealed by sum-frequency
generation spectroscopy, the vibrational structure of ligands is critically correlated to QDs
electronic structure when these are pumped into their excitonic states. Given the different
hypotheses commonly put forward, such a correlation is expected to derive from either a
direct overlap between the electronic wavefunctions, a charge transfer, or an energy transfer.
Assuming that the polarizability of ligands is subordinate to the local electric field induced by
excitons through dipolar interaction, our classical model based on nonlinear optics unambiguously
supports the latter hypothesis.
Disciplines :
Physics
Author, co-author :
Noblet, Thomas ; Université Paris-Sud 11 > laboratoire de Chimie Physique
Dreesen, Laurent ; Université de Liège - ULiège > Département de physique > Biophotonique
Boujday, Souhir; Université Paris-Sorbonne (Paris IV) > Laboratoire de Réactivité de Surface
Méthivier, Christophe; Université Paris-Sorbonne (Paris IV) > Laboratoire de Réactivité de Surface
Busson, Bertrand; Université Paris-Sud 11 > Laboratoire de Chimie Physique
Tadjeddine, A.; Université Paris-Sud 11 > Laboratoire de Chimie Physique
Humbert, Christophe; Université Paris-Sud 11 > Laboratoire de Chimie Physique
Language :
English
Title :
Semiconductor quantum dots reveal dipolar coupling from exciton to ligand vibration
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