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Coupled colloidal quantum dot molecules composed of two fused CdSe/CdScore/shell sphere monomers were recently presented. Upon fusion, the potentialenergy landscape is changing into two quantum dots separated by a pre-tunedpotential barrier with energetics dictated by the conduction and valence bandoffsets of the core/shell semiconductors, and width controlled by the shellthickness and the fusion reaction conditions. In close proximity of the twonanocrystals, orbital hybridization occurs, forming bonding and anti-bondingstates in analogy to the hydrogen molecule. In this study, we examinetheoretically the electronic and optical signatures of such a quantum dot dimercompared to its monomer core/shell building blocks. We examine the effects ofdifferent core sizes, barrier widths, different band offsets and neck sizes atthe interface of the fused facets, on the system wave-functions and energetics.Due to the higher effective mass of the hole and the large valence band offset,the hole still essentially resides in either of the cores breaking the symmetryof the potential for the electron as well. We found that the dimer signature iswell expressed in a redshift of the bandgap both in absorption and emission, inslower radiative lifetimes and in an absorption cross-section which issignificantly enhanced relative to the monomers at energies above the shellabsorption onset, while remains essentially at the same level near theband-edge. This study provides essential guidance to pre-design of coupledquantum dot molecules with specific attributes which can be utilized forvarious new optoelectronic applications.

Electronic coupling in colloidal quantum dot molecules; The case of CdSe/CdS core/shell homodimers