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Understanding how carbon dioxide (CO2) behaves and interacts with surfaces is paramount for the development of sensors and materials to attempt CO2 mitigation and catalysis. Here, we combine simultaneous atomic force microscopy (AFM) and scanning tunneling microscopy (STM) using CO-functionalized probes with density functional theory (DFT)-based simulations to gain fundamental insight into the behavior of physisorbed CO2 molecules on a gold(111) surface that also contains one-dimensional metal−organic chains formed by 1,4-15 phenylene diisocyanide (PDI) bridged by gold (Au) adatoms. We resolve the structure of self-assembled CO2 islands, both confined between the PDI−Au chains as well as free-standing on the surface and reveal a chiral arrangement of CO2 molecules in a windmill-like structure that encloses a standing-up CO2 molecule and other foreign species existing at the surface. We identify these species by the comparison of height-dependent AFM and STM imaging with DFT-calculated images and clarify the origin of the kagome tiling exhibited by this surface system. Our results show the complementarity of AFM and STM using functionalized probes and their potential, when combined with DFT, to explore greenhouse gas molecules at surface-supported model systems.

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• In Copyright
  

  This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsnano.4c07034

Keyword: CO2 islands, 1,4-phenylene diisocyanide, chirality, metal organic chains, atomic force microscopy, scanning tunneling microscopy, density functional theory

Date published: 2024-10-01

Publisher: American Chemical Society (ACS)

Journal:

• ACS Nano (ISSN: 19360851) vol. 18 issue. 39 p. 26759-26769

Funding:

• Ministry of Education, Culture, Sports, Science and Technology 21H01812
• Ministry of Education, Culture, Sports, Science and Technology 21K18876
• Ministry of Education, Culture, Sports, Science and Technology 24K01350
• Ministry of Education, Culture, Sports, Science and Technology 24K21716
• Ministry of Education, Culture, Sports, Science and Technology PE16046
• Ministerio de Ciencia, Tecnología e Innovación Productiva CEX2018-000805-M
• Ministerio de Ciencia, Tecnología e Innovación Productiva CEX2023-001316-M
• Ministerio de Ciencia, Tecnología e Innovación Productiva PID2020-115864RB-I00
• Ministerio de Ciencia, Tecnología e Innovación Productiva RYC2021-031176-I
• Ministerio de Ciencia, Tecnología e Innovación Productiva TED2021-132219A-I00
• Ministry of Education, Culture, Sports, Science and Technology AM2100 (National Institute for Materials Science (NIMS))
• Ministry of Education, Culture, Sports, Science and Technology 19H05789
• Ministry of Education, Culture, Sports, Science and Technology 22H00285
• Ministry of Education, Culture, Sports, Science and Technology AG2030 (National Institute for Materials Science (NIMS))

Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4795

First published URL: https://doi.org/10.1021/acsnano.4c07034

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Updated at: 2025-09-17 08:30:31 +0900

Published on MDR: 2025-09-17 08:21:53 +0900