Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 10, Pages 4522-4529Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c12618
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Funding
- MCIN/AEI [PID2019-107338RBC61, PID2019-107338RB-C62, PID2019-107338RB-C63, PID2019-109555GB-I00, FJC2019-041202-I]
- Basque Government [IT-1255-19, PIBA19-0004]
- Spanish Research Council [ILINKC20002]
- European Union [863098, 101022150]
- Xunta de Galicia (Centro Singular de Investigacion de Galicia, 2019-2022) [ED431G2019/03]
- Marie Curie Actions (MSCA) [101022150] Funding Source: Marie Curie Actions (MSCA)
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This study successfully synthesized nitrogen-doped triangulene and characterized its electronic properties through experimental and theoretical calculations. It was demonstrated that nitrogen-doped triangulene exhibits an open-shell triplet ground state on Au(111) surface and a closed-shell character on Ag(111) surface.
Nitrogen heteroatom doping into a triangulene molecule allows tuning its magnetic state. However, the synthesis of the nitrogen-doped triangulene (aza-triangulene) has been challenging. Herein, we report the successful synthesis of aza-triangulene on the Au(111) and Ag(111) surfaces, along with their characterizations by scanning tunneling microscopy and spectroscopy in combination with density functional theory (DFT) calculations. Aza-triangulenes were obtained by reducing ketone-substituted precursors. Exposure to atomic hydrogen followed by thermal annealing and, when necessary, manipulations with the scanning probe afforded the target product. We demonstrate that on Au(111), aza-triangulene donates an electron to the substrate and exhibits an open-shell triplet ground state. This is derived from the different Kondo resonances of the final aza-triangulene product and a series of intermediates on Au(111). Experimentally mapped molecular orbitals match with DFT-calculated counterparts for a positively charged aza-triangulene. In contrast, aza-triangulene on Ag(111) receives an extra electron from the substrate and displays a closed-shell character. Our study reveals the electronic properties of aza-triangulene on different metal surfaces and offers an approach for the fabrication of new hydrocarbon structures, including reactive open-shell molecules.
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