| Autor: |
Kawai, Shigeki, Silveira, Orlando J., Kurki, Lauri, Yuan, Zhangyu, Nishiuchi, Tomohiko, Kodama, Takuya, Sun, Kewei, Custance, Oscar, Lado, Jose L., Kubo, Takashi, Foster, Adam S. |
| Rok vydání: |
2023 |
| Předmět: |
|
| Druh dokumentu: |
Working Paper |
| DOI: |
10.1038/s41467-023-43659-4 |
| Popis: |
Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has a great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state. |
| Databáze: |
arXiv |
| Externí odkaz: |
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