On-Surface Synthesis and Determination of the Open-Shell Singlet Ground State of Tridecacene
Status PubMed-not-MEDLINE Jazyk angličtina Země Německo Médium print-electronic
Typ dokumentu časopisecké články
Grantová podpora
2017/26/E/ST3/00855
Narodowe Centrum Nauki
23-05486S
Grantová Agentura České Republiky
CEX2019-000925- S
Ministerio de Ciencia, Innovación y Universidades
PID2019-104815GB-I00
Ministerio de Ciencia, Innovación y Universidades
CERCA Program
Departament de Salut, Generalitat de Catalunya
LM2023051
Ministerstvo Školství, Mládeže a Tělovýchovy
Large Infrastructures for Research
Ministerstvo Školství, Mládeže a Tělovýchovy
PubMed
38192200
DOI
10.1002/anie.202317091
Knihovny.cz E-zdroje
- Klíčová slova
- Diradicals, Higher Acenes, Inelastic Excitation, Many-Body Calculations, Open-Shell Compounds,
- Publikační typ
- časopisecké články MeSH
The character of the electronic structure of acenes has been the subject of longstanding discussion. However, convincing experimental evidence of their open-shell character has so far been missing. Here, we present the on-surface synthesis of tridecacene molecules by thermal annealing of octahydrotridecacene on a Au(111) surface. We characterized the electronic structure of the tridecacene by scanning probe microscopy, which reveals the presence of an inelastic signal at 126 meV. We attribute the inelastic signal to spin excitation from the singlet diradical ground state to the triplet excited state. To rationalize the experimental findings, we carried out many-body ab initio calculations as well as model Hamiltonians to take into account the effect of the metallic substrate. Moreover, we provide a detailed analysis of how the dynamic electron correlation and virtual charge fluctuation between the molecule and metallic surface reduces the singlet-triplet band gap. Thus, this work provides the first experimental confirmation of the magnetic character of tridecacene.
Departament de Quımica Organica i Analıtica Universitat Rovira i Virgili 43007 Tarragona Spain
Institute of Physics Lodz University of Technology ul Wolczanska 219 90924 Lodz Poland
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