Bistability between $π$-diradical open-shell and closed-shell states in indeno[1,2-a]fluorene

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Auteurs principaux: Mishra, Shantanu, Vilas-Varela, Manuel, Lieske, Leonard-Alexander, Ortiz, Ricardo, Fatayer, Shadi, Rončević, Igor, Albrecht, Florian, Frederiksen, Thomas, Peña, Diego, Gross, Leo
Format: Preprint
Publié: 2023
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author Mishra, Shantanu
Vilas-Varela, Manuel
Lieske, Leonard-Alexander
Ortiz, Ricardo
Fatayer, Shadi
Rončević, Igor
Albrecht, Florian
Frederiksen, Thomas
Peña, Diego
Gross, Leo
author_facet Mishra, Shantanu
Vilas-Varela, Manuel
Lieske, Leonard-Alexander
Ortiz, Ricardo
Fatayer, Shadi
Rončević, Igor
Albrecht, Florian
Frederiksen, Thomas
Peña, Diego
Gross, Leo
contents Indenofluorenes are non-benzenoid conjugated hydrocarbons that have received great interest owing to their unusual electronic structure and potential applications in non-linear optics and photovoltaics. Here, we report the generation of unsubstituted indeno[1,2-a]fluorene, the final and yet unreported parent indenofluorene isomer, on various surfaces by cleavage of two C-H bonds in 7,12-dihydroindeno[1,2-a]fluorene through voltage pulses applied by the tip of a combined scanning tunneling microscope and atomic force microscope. On bilayer NaCl on Au(111), indeno[1,2-a]fluorene is in the neutral charge state, while it exhibits charge bistability between neutral and anionic states on the lower work function surfaces of bilayer NaCl on Ag(111) and Cu(111). In the neutral state, indeno[1,2-a]fluorene exhibits either of two ground states: an open-shell pi-diradical state, predicted to be a triplet by density functional and multireference many-body perturbation theory calculations, or a closed-shell state with a para-quinodimethane moiety in the as-indacene core. Switching between open- and closed-shell states of a single molecule is observed by changing its adsorption site on NaCl.
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id arxiv_https___arxiv_org_abs_2303_04483
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Bistability between $π$-diradical open-shell and closed-shell states in indeno[1,2-a]fluorene
Mishra, Shantanu
Vilas-Varela, Manuel
Lieske, Leonard-Alexander
Ortiz, Ricardo
Fatayer, Shadi
Rončević, Igor
Albrecht, Florian
Frederiksen, Thomas
Peña, Diego
Gross, Leo
Mesoscale and Nanoscale Physics
Indenofluorenes are non-benzenoid conjugated hydrocarbons that have received great interest owing to their unusual electronic structure and potential applications in non-linear optics and photovoltaics. Here, we report the generation of unsubstituted indeno[1,2-a]fluorene, the final and yet unreported parent indenofluorene isomer, on various surfaces by cleavage of two C-H bonds in 7,12-dihydroindeno[1,2-a]fluorene through voltage pulses applied by the tip of a combined scanning tunneling microscope and atomic force microscope. On bilayer NaCl on Au(111), indeno[1,2-a]fluorene is in the neutral charge state, while it exhibits charge bistability between neutral and anionic states on the lower work function surfaces of bilayer NaCl on Ag(111) and Cu(111). In the neutral state, indeno[1,2-a]fluorene exhibits either of two ground states: an open-shell pi-diradical state, predicted to be a triplet by density functional and multireference many-body perturbation theory calculations, or a closed-shell state with a para-quinodimethane moiety in the as-indacene core. Switching between open- and closed-shell states of a single molecule is observed by changing its adsorption site on NaCl.
title Bistability between $π$-diradical open-shell and closed-shell states in indeno[1,2-a]fluorene
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2303.04483