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We investigate the charge re-distribution upon optical excitation of variousnecked homodimer CQDMs using single particle emission spectroscopy. By tuningthe hybridization of the electron wavefunction at a fixed center-to-centerdistance through controlling the neck girth, we reveal two coupling limits. Onone hand a connected-but-confined situation where neighbouring CQDs are weaklyfused to each other manifesting a weak coupling regime, and on the other hand,a connected-and-delocalized situation, where the neck is filled beyond thefacet size leading to a rod-like architecture manifesting strong-coupling.Either coupling regimes entrust distinct optical signatures clearly resolved atroom temperature in terms of photoluminescence quantum yield, intensity timetraces, lifetimes, and spectra of the neutral-exciton, charged-exciton, andbiexciton states. The interplay between the radiative and non-radiative Augerdecays of these states, turns emitted photons from the CQDMs in theweak-coupling regime highly bunched unlike CQD monomers, while the antibunchingis regained at the strong-coupling regime. This behavior correlates with thehybridization energy being smaller than the thermal energy (kT approx. 25meV)at the weak-coupling limit (delta E approax.5-10meV), leading to excitonlocalization suppressing Auger decay. In the neck-filled architectures, thelarger hybridization energy (delta E approx.20-30meV) leads to excitondelocalization while activating the fast charged and multi-exciton Auger decayprocesses. This work sets an analogy for the artificial molecule CQDMs withregular molecules, where the two distinct regimes of weak- and strong-couplingcorrespond to ionic- or covalent- type bonding, respectively.

Photon Correlations in Colloidal Quantum Dot Molecules Controlled by the Neck Barrier