\"Darker-than-Black\" PbS Quantum Dots: Enhancing Optical Absorption of Colloidal Semiconductor Nanocrystals via Short Conjugated Ligands. (Articolo in rivista)

Type
Label
  • \"Darker-than-Black\" PbS Quantum Dots: Enhancing Optical Absorption of Colloidal Semiconductor Nanocrystals via Short Conjugated Ligands. (Articolo in rivista) (literal)
Anno
  • 2015-01-01T00:00:00+01:00 (literal)
Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#doi
  • 10.1021/ja510739q (literal)
Alternative label
  • Giansante, Carlo; Infante, Ivan; Fabiano, Eduardo; Grisorio, Roberto; Suranna, Gian Paolo; Gigli, Giuseppe (2015)
    "Darker-than-Black" PbS Quantum Dots: Enhancing Optical Absorption of Colloidal Semiconductor Nanocrystals via Short Conjugated Ligands.
    in Journal of the Chemical Society. Dalton transactions (Print)
    (literal)
Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#autori
  • Giansante, Carlo; Infante, Ivan; Fabiano, Eduardo; Grisorio, Roberto; Suranna, Gian Paolo; Gigli, Giuseppe (literal)
Pagina inizio
  • 1875 (literal)
Pagina fine
  • 86 (literal)
Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#url
  • http://dx.doi.org/10.1021/ja510739q (literal)
Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#numeroVolume
  • 137 (literal)
Rivista
Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#numeroFascicolo
  • 5 (literal)
Note
  • ISI Web of Science (WOS) (literal)
Http://www.cnr.it/ontology/cnr/pubblicazioni.owl#affiliazioni
  • Center for Biomolecular Nanotechnologies @UNILE, Istituto Italiano di Tecnologia, via Barsanti 1, 73010 Arnesano, Lecce, Italy NNL-CNR Istituto di Nanoscienze, via per Arnesano, 73100 Lecce, Lecce, Italy Kimika Fakultatea, Euskal Herriko Unibersitatea and Donostia International Physics Center (DIPC), CP1072, 20080 San Sebastian, Spain Department of Theoretical Chemistry, Faculty of Sciences, Vrije Universiteit Amsterdam, De Boelelaan 1083, 1081 HV Amsterdam, The Netherlands (literal)
Titolo
  • \"Darker-than-Black\" PbS Quantum Dots: Enhancing Optical Absorption of Colloidal Semiconductor Nanocrystals via Short Conjugated Ligands. (literal)
Abstract
  • Colloidal quantum dots (QDs) stand among the most attractive light-harvesting materials to be exploited for solution-processed optoelectronic applications. To this aim, quantitative replacement of the bulky electrically insulating ligands at the QD surface coming from the synthetic procedure is mandatory. Here we present a conceptually novel approach to design light-harvesting nanomaterials demonstrating that QD surface modification with suitable short conjugated organic molecules permits us to drastically enhance light absorption of QDs, while preserving good long-term colloidal stability. Indeed, rational design of the pendant and anchoring moieties, which constitute the replacing ligand framework leads to a broadband increase of the optical absorbance larger than 300% for colloidal PbS QDs also at high energies (>3.1 eV), which could not be predicted by using formalisms derived from effective medium theory. We attribute such a drastic absorbance increase to ground-state ligand/QD orbital mixing, as inferred by density functional theory calculations; in addition, our findings suggest that the optical band gap reduction commonly observed for PbS QD solids treated with thiol-terminating ligands can be prevalently ascribed to 3p orbitals localized on anchoring sulfur atoms, which mix with the highest occupied states of the QDs. More broadly, we provide evidence that organic ligands and inorganic cores are inherently electronically coupled materials thus yielding peculiar chemical species (the colloidal QDs themselves), which display arising (opto)electronic properties that cannot be merely described as the sum of those of the ligand and core components. (literal)
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