Actinide Coordination Chemistry on Surfaces: Synthesis, Manipulation, and Properties of Thorium Bis(porphyrinato) Complexes - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of the American Chemical Society Année : 2021

Actinide Coordination Chemistry on Surfaces: Synthesis, Manipulation, and Properties of Thorium Bis(porphyrinato) Complexes

Erik Rheinfrank
  • Fonction : Auteur
Mathias Pörtner
  • Fonction : Auteur
Felix Haag
  • Fonction : Auteur
Peter S Deimel
  • Fonction : Auteur
Francesco Allegretti
Knud Seufert
Johannes V Barth
Marie-Laure Bocquet
Peter Feulner
  • Fonction : Auteur
Willi Auwärter

Résumé

Actinide-based metal−organic complexes and coordination architectures encompass intriguing properties and functionalities but are still largely unexplored on surfaces. We introduce the in situ synthesis of actinide tetrapyrrole complexes under ultrahighvacuum conditions, on both a metallic support and a 2D material. Specifically, exposure of a tetraphenylporphyrin (TPP) multilayer to an elemental beam of thorium followed by a temperatureprogrammed reaction and desorption of surplus molecules yields bis(porphyrinato)thorium (Th(TPP) 2) assemblies on Ag(111) and hexagonal boron nitride/Cu(111). A multimethod characterization including X-ray photoelectron spectroscopy, scanning tunneling microscopy, temperature-programmed desorption, and complementary density functional theory modeling provides insights into conformational and electronic properties. Supramolecular assemblies of Th(TPP) 2 as well as individual doubledeckers are addressed with submolecular precision, e.g., demonstrating the reversible rotation of the top porphyrin in Th(TPP) 2 by molecular manipulation. Our findings thus demonstrate prospects for actinide-based functional nanoarchitectures.

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Dates et versions

hal-03432277 , version 1 (17-11-2021)

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Erik Rheinfrank, Mathias Pörtner, Maria del Carmen Nuñez Beyerle, Felix Haag, Peter S Deimel, et al.. Actinide Coordination Chemistry on Surfaces: Synthesis, Manipulation, and Properties of Thorium Bis(porphyrinato) Complexes. Journal of the American Chemical Society, 2021, 143 (36), pp.14581-14591. ⟨10.1021/jacs.1c04982⟩. ⟨hal-03432277⟩
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