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Optical Images of M...
Optical Images of Molecular Vibronic Couplings from Tip-Enhanced Fluorescence Excitation SpectroscopyY
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- Qiu, Feifei (author)
- Yanshan Univ, Sch Sci, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Hebei, Peoples R China.;Yanshan Univ, Sch Sci, Key Lab Microstruct Mat Phys Hebei Prov, Qinhuangdao 066004, Hebei, Peoples R China.
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- Gong, Zu-Yong (author)
- Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, MOE Key Lab Computat Phys Sci,Dept Chem, Shanghai 200433, Peoples R China.
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- Cao, Dongwei (author)
- Yanshan Univ, Sch Sci, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Hebei, Peoples R China.;Yanshan Univ, Sch Sci, Key Lab Microstruct Mat Phys Hebei Prov, Qinhuangdao 066004, Hebei, Peoples R China.
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- Song, Ce (author)
- KTH,Teoretisk kemi och biologi,Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China.;Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China
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- Tian, Guangjun (author)
- Yanshan Univ, Sch Sci, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Hebei, Peoples R China.;Yanshan Univ, Sch Sci, Key Lab Microstruct Mat Phys Hebei Prov, Qinhuangdao 066004, Hebei, Peoples R China.
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- Duan, Sai (author)
- Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, MOE Key Lab Computat Phys Sci,Dept Chem, Shanghai 200433, Peoples R China.
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- Luo, Yi (author)
- Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China.;Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China.
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Yanshan Univ, Sch Sci, State Key Lab Metastable Mat Sci & Technol, Qinhuangdao 066004, Hebei, Peoples R China;Yanshan Univ, Sch Sci, Key Lab Microstruct Mat Phys Hebei Prov, Qinhuangdao 066004, Hebei, Peoples R China. Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, MOE Key Lab Computat Phys Sci,Dept Chem, Shanghai 200433, Peoples R China. (creator_code:org_t)
- 2021-12-23
- 2022
- English.
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In: JACS Au. - : American Chemical Society (ACS). - 2691-3704. ; 2:1, s. 150-158
- Related links:
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https://doi.org/10.1...
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https://pubs.acs.org...
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https://urn.kb.se/re...
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Abstract
Subject headings
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- Tip-based photoemission spectroscopic techniques have now achieved subnanometer resolution that allows visualization of the chemical structure and even the ground-state vibrational modes of a single molecule. However, the ability to visualize the interplay between electronic and nuclear motions of excited states, i.e., vibronic couplings, is yet to be explored. Herein, we theoretically propose a new technique, namely, tip-enhanced fluorescence excitation (TEFE). TEFE takes advantage of the highly confined plasmonic field and thus can offer a possibility to directly visualize the vibronic effect of a single molecule in real space for arbitrary excited states in a given energy window. Numerical simulations for a single porphine molecule confirm that vibronic couplings originating from Herzberg-Teller (HT) active modes can be visually identified. TEFE further enables high-order vibrational transitions that are normally suppressed in the other plasmon-based processes. Images of the combination vibrational transitions have the same pattern as that of their parental HT active mode's fundamental transition, providing a direct protocol for measurements of the activity of Franck-Condon modes of selected excited states. These findings strongly suggest that TEFE is a powerful strategy to identify the involvement of molecular moieties in the complicated electron-nuclear interactions of the excited states at the single-molecule level.
Subject headings
- NATURVETENSKAP -- Kemi -- Teoretisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Theoretical Chemistry (hsv//eng)
Keyword
- vibronic coupling
- tip-enhanced fluorescence excitation
- single-molecule imaging
- plasmonic field
- Franck-Condon activity
Publication and Content Type
- ref (subject category)
- art (subject category)
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