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Using Spectator Ligands to Enhance Nanocrystal-to-Molecule Electron Transfer.
Raulerson, Emily K; Cadena, Danielle M; Jabed, Mohammed A; Wight, Christopher D; Lee, Inki; Wagner, Holden R; Brewster, James T; Iverson, Brent L; Kilina, Svetlana; Roberts, Sean T.
Afiliação
  • Raulerson EK; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Cadena DM; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Jabed MA; Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58108, United States.
  • Wight CD; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Lee I; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Wagner HR; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Brewster JT; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Iverson BL; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
  • Kilina S; Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58108, United States.
  • Roberts ST; Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
J Phys Chem Lett ; 13(6): 1416-1423, 2022 Feb 17.
Article em En | MEDLINE | ID: mdl-35119280
Semiconductor nanocrystals (NCs) have emerged as promising photocatalysts. However, NCs are often functionalized with complex ligand shells that contain not only charge acceptors but also other "spectator ligands" that control NC solubility and affinity for target reactants. Here, we show that spectator ligands are not passive observers of photoinduced charge transfer but rather play an active role in this process. We find the rate of electron transfer from quantum-confined PbS NCs to perylenediimide acceptors can be varied by over a factor of 4 simply by coordinating cinnamate ligands with distinct dipole moments to NC surfaces. Theoretical calculations indicate this rate variation stems from both ligand-induced changes in the free energy for charge transfer and electrostatic interactions that alter perylenediimide electron acceptor orientation on NC surfaces. Our work shows NC-to-molecule charge transfer can be fine-tuned through ligand shell design, giving researchers an additional handle for enhancing NC photocatalysis.

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2022 Tipo de documento: Article

Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2022 Tipo de documento: Article