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Open Access Publications from the University of California

PbS nanoparticles capped with tetrathiafulvalenetetracarboxylate: utilizing energy level alignment for efficient carrier transport.

  • Author(s): Scheele, Marcus
  • Hanifi, David
  • Zherebetskyy, Danylo
  • Chourou, Slim T
  • Axnanda, Stephanus
  • Rancatore, Benjamin J
  • Thorkelsson, Kari
  • Xu, Ting
  • Liu, Zhi
  • Wang, Lin-Wang
  • Liu, Yi
  • Alivisatos, A Paul
  • et al.

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We fabricate a field-effect transistor by covalently functionalizing PbS nanoparticles with tetrathiafulvalenetetracarboxylate. Following experimental results from cyclic voltammetry and ambient-pressure X-ray photoelectron spectroscopy, we postulate a near-resonant alignment of the PbS 1Sh state and the organic HOMO, which is confirmed by atomistic calculations. Considering the large width of interparticle spacing, we observe an abnormally high field-effect hole mobility, which we attribute to the postulated resonance. In contrast to nanoparticle devices coupled through common short-chained ligands, our system maintains a large degree of macroscopic order as revealed by X-ray scattering. This provides a different approach to the design of hybrid organic-inorganic nanomaterials, circumvents the problem of phase segregation, and holds for versatile ways to design ordered, coupled nanoparticle thin films.

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