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@ARTICLE{Marino:885445,
      author       = {Marino, Emanuele and Sciortino, Alice and Berkhout,
                      Annemarie and MacArthur, Katherine E. and Heggen, Marc and
                      Gregorkiewicz, Tom and Kodger, Thomas E. and Capretti,
                      Antonio and Murray, Christopher B. and Koenderink, A. Femius
                      and Messina, Fabrizio and Schall, Peter},
      title        = {{S}imultaneous {P}hotonic and {E}xcitonic {C}oupling in
                      {S}pherical {Q}uantum {D}ot {S}upercrystals},
      journal      = {ACS nano},
      volume       = {14},
      issn         = {1936-086X},
      address      = {Washington, DC},
      publisher    = {Soc.},
      reportid     = {FZJ-2020-03828},
      pages        = {13806-13815},
      year         = {2020},
      abstract     = {Semiconductor nanocrystals, or quantum dots (QDs),
                      simultaneously benefit from inexpensive low-temperature
                      solution processing and exciting photophysics, making them
                      the ideal candidates for next-generation solar cells and
                      photodetectors. While the working principles of these
                      devices rely on light absorption, QDs intrinsically belong
                      to the Rayleigh regime and display optical behavior limited
                      to electric dipole resonances, resulting in low absorption
                      efficiencies. Increasing the absorption efficiency of QDs,
                      together with their electronic and excitonic coupling to
                      enhance charge carrier mobility, is therefore of critical
                      importance to enable practical applications. Here, we
                      demonstrate a general and scalable approach to increase both
                      light absorption and excitonic coupling of QDs by
                      fabricating hierarchical metamaterials. We assemble QDs into
                      crystalline supraparticles using an emulsion template and
                      demonstrate that these colloidal supercrystals (SCs) exhibit
                      extended resonant optical behavior resulting in an
                      enhancement in absorption efficiency in the visible range of
                      more than 2 orders of magnitude with respect to the case of
                      dispersed QDs. This successful light trapping strategy is
                      complemented by the enhanced excitonic coupling observed in
                      ligand-exchanged SCs, experimentally demonstrated through
                      ultrafast transient absorption spectroscopy and leading to
                      the formation of a free biexciton system on sub-picosecond
                      time scales. These results introduce a colloidal
                      metamaterial designed by self-assembly from the bottom up,
                      simultaneously featuring a combination of nanoscale and
                      mesoscale properties leading to simultaneous photonic and
                      excitonic coupling, therefore presenting the nanocrystal
                      analogue of supramolecular structures.},
      cin          = {ER-C-1},
      ddc          = {540},
      cid          = {I:(DE-Juel1)ER-C-1-20170209},
      pnm          = {143 - Controlling Configuration-Based Phenomena (POF3-143)},
      pid          = {G:(DE-HGF)POF3-143},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {pmid:32924433},
      UT           = {WOS:000586793400128},
      doi          = {10.1021/acsnano.0c06188},
      url          = {https://juser.fz-juelich.de/record/885445},
}