Tunable exciton binding energy in 2D hybrid layered perovskites through donor-acceptor interactions within the organic layer.

Autor: Passarelli JV; Department of Chemistry, Northwestern University, Evanston, IL, USA., Mauck CM; Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA.; Department of Chemistry, Kenyon College, Gambier, OH, USA., Winslow SW; Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA., Perkinson CF; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA., Bard JC; Department of Chemistry, Northwestern University, Evanston, IL, USA., Sai H; Simpson Querrey Institute, Northwestern University, Chicago, IL, USA., Williams KW; Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA., Narayanan A; Simpson Querrey Institute, Northwestern University, Chicago, IL, USA., Fairfield DJ; Department of Materials Science and Engineering, Northwestern University, Evanston, IL, USA., Hendricks MP; Simpson Querrey Institute, Northwestern University, Chicago, IL, USA., Tisdale WA; Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA. tisdale@mit.edu., Stupp SI; Department of Chemistry, Northwestern University, Evanston, IL, USA. s-stupp@northwestern.edu.; Simpson Querrey Institute, Northwestern University, Chicago, IL, USA. s-stupp@northwestern.edu.; Department of Materials Science and Engineering, Northwestern University, Evanston, IL, USA. s-stupp@northwestern.edu.; Department of Biomedical Engineering, Northwestern University, Evanston, IL, USA. s-stupp@northwestern.edu.; Department of Medicine, Northwestern University, Chicago, IL, USA. s-stupp@northwestern.edu.
Jazyk: angličtina
Zdroj: Nature chemistry [Nat Chem] 2020 Aug; Vol. 12 (8), pp. 672-682. Date of Electronic Publication: 2020 Jul 06.
DOI: 10.1038/s41557-020-0488-2
Abstrakt: The strength of electrostatic interactions within semiconductors strongly affects their performance in optoelectronic devices. An important target is the tuning of a material's exciton binding energy-the energy binding an electron-hole pair through the electrostatic Coulomb force-independent of its electronic band gap. Here, we report on the doping of a family of two-dimensional hybrid perovskites, in which inorganic lead halide sheets alternate with naphthalene-based organic layers, with tetrachloro-1,2-benzoquinone (TCBQ). For four out of seven n = 1 perovskites, the incorporation of the electron-accepting TCBQ dopant into the organic sublattice containing the electron-donating naphthalene species enabled the tuning of the materials' 1s exciton binding energy. The naphthalene-TCBQ electron donor-acceptor interactions increased the electrostatic screening of the exciton, in turn lowering its binding energy relative to the undoped perovskite-by almost 50% in one system. Structural and optical characterization showed that the inorganic lattice is not significantly perturbed even though the layer-to-layer spacing increases upon molecular dopant incorporation.
Databáze: MEDLINE
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