Photon correlations in colloidal quantum dot molecules controlled by the neck barrier

Somnath Koley, Jiabin Cui, Yossef E. Panfil, Yonatan Ossia, Adar Levi, Einav Scharf, Lior Verbitsky, Uri Banin*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

The charge redistribution upon optical excitation of various necked homodimer colloidal quantum dot molecules (CQDMs) is investigated using single-particle emission spectroscopy. By tuning the hybridization of the electron wavefunctions at a fixed center-to-center distance through controlling the neck girth, we reveal two coupling limits: on one hand, a “connected-but-confined” situation where neighboring CQDs are weakly fused to each other, manifesting a weak-coupling regime, and on the other hand, a “connected-and-delocalized” situation where the neck is filled beyond the facet size, leading to a rod-like architecture manifesting strong coupling. The interplay between the radiative and non-radiative Auger decays of these states turns emitted photons from the CQDMs in the weak-coupling regime highly bunched unlike CQD monomers, while the antibunching is regained at the strong-coupling regime. This work sets an analogy for the artificial molecule CQDMs with regular molecules, where the two distinct regimes of weak and strong coupling correspond to ionic- or covalent-type bonding, respectively.

Original languageAmerican English
Pages (from-to)3997-4014
Number of pages18
JournalMatter
Volume5
Issue number11
DOIs
StatePublished - 2 Nov 2022

Bibliographical note

Publisher Copyright:
© 2022 Elsevier Inc.

Keywords

  • Auger process
  • MAP2: Benchmark
  • colloidal quantum dots
  • electronic coupling
  • photon antibunching
  • single-particle spectroscopy

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