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Competing Intermolecular and Molecule-Surface Interactions: Dipole-Dipole-Driven Patterns in Mixed Carborane Self-Assembled Monolayers
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SYSNO ASEP 0584549 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Competing Intermolecular and Molecule-Surface Interactions: Dipole-Dipole-Driven Patterns in Mixed Carborane Self-Assembled Monolayers Author(s) White, K. E. (US)
Avery, E. (US)
Cummings, E. (US)
Hong, Z. (US)
Langecker, Jens (UACH-T) SAI
Vetushka, Aliaksi (FZU-D) RID, ORCID
Dušek, Michal (FZU-D) RID, ORCID, SAI
Macháček, Jan (UACH-T) RID, ORCID, SAI
Višňák, Jakub (UACH-T) ORCID, RID, SAI
Endres, J. (CZ)
Bastl, Zdeněk (UFCH-W) RID, ORCID
Mete, E. (TR)
Alexandrova, A. N. (US)
Baše, Tomáš (UACH-T) RID, SAI, ORCID
Weiss, P. S. (US)Number of authors 15 Source Title Chemistry of Materials. - : American Chemical Society - ISSN 0897-4756
Roč. 36, č. 4 (2024), s. 2085-2095Number of pages 11 s. Language eng - English Country US - United States Keywords Molecular interactions ; Molecules ; Molecular structure ; Scanning tunneling microscopy ; Supramolecular chemistry Subject RIV CA - Inorganic Chemistry OECD category Inorganic and nuclear chemistry R&D Projects LTAIN19152 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) EF16_026/0008382 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) LM2018096 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) Research Infrastructure e-INFRA CZ - 90140 - CESNET, zájmové sdružení právnických osob Method of publishing Limited access Institutional support UACH-T - RVO:61388980 ; FZU-D - RVO:68378271 ; UFCH-W - RVO:61388955 UT WOS 001166534100001 EID SCOPUS 85186165727 DOI 10.1021/acs.chemmater.3c03210 Annotation Carboranedithiol isomers adsorbing with opposite orientations of their dipoles on surfaces are self-assembled together to form mixed monolayers where both lateral dipole-dipole and lateral thiol-thiolate (S-H···S) interactions provide enhanced stability over single-component monolayers. We demonstrate the first instance of the ability to map individual isomers in a mixed monolayer using the model system carboranedithiols on Au{111}. The addition of methyl groups to one isomer provides both an enhanced dipole moment and extra apparent height for differentiation via scanning tunneling microscopy (STM). Associated computational investigations rationalize favorable interactions of mixed pairs and the associated stability changes that arise from these interactions. Both STM images and Monte Carlo simulations yield similarly structured mixed monolayers, where approximately 10% of the molecules have reversed dipole moment orientations but no direct chemical attachment to the surface, leading to homogeneous monolayers with no apparent phase separation. Deprotonating the thiols by depositing the molecules under basic conditions eliminates the lateral S-H···S interactions while accentuating the dipole-dipole forces. The molecular system investigated is composed of isomeric molecules with opposite orientations of dipoles and identical surface packing, which enables the mapping of individual molecules within the mixed monolayers and enables analyses of the contributions of the relatively weak lateral interactions to the overall stability of the assemblies. Workplace Institute of Inorganic Chemistry Contact Jana Kroneislová, krone@iic.cas.cz, Tel.: 311 236 931 Year of Publishing 2025 Electronic address https://pubs.acs.org/doi/10.1021/acs.chemmater.3c03210
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