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Role of Core-Shell Formation in Exciton Confinement Relaxation in Dithiocarbamate-Capped CdSe QDs.
Journal of Physical Chemistry Letters 2017 July 21
The possibility of exciton delocalization in alkyldithiocarbamate (ATC)-capped CdSe has been investigated for several alkyl groups and compared with phenyldithiocarbamates (PTCs). We find a bathochromic shift for ATC similar to the one obtained for PTC. Our computational studies show reduction in HOMO-LUMO gaps in both PTC and ATC, albeit with a lower shift. However, TDDFT studies revealed that ATC-capped CdSe is more of a localized HOMO state as compared with partly delocalized HOMO in PTC-capped CdSe, hinting at a difference in electronic interaction between the two binding groups. We hypothesized the formation of sulfide layer over the CdSe QDs as the possible reason for the observed bathochromic shift, as verified by absorption spectra of S2- ligand exchange samples. The formation of CdS shell leads to substantial electron delocalization because CdSe CB is in close resonance with CdS, which is exactly the opposite of what was previously concluded in the literature.
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