Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 4, Issue 20, Pages 3413-3419Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz4016124
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Funding
- Nebraska Center for Energy Sciences Research
- National Science Foundation through the Materials Research Science and Engineering Center [DMR-0213808]
- National Science Foundation [EPS-1004094]
- Center for Computational Research at the University at Buffalo
- European Union through the Foundation for Polish Science (HOMING Plus program)
- Alfred P. Sloan Foundation
- Department of Defense [W911NF-12-1-0080]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [0747704] Funding Source: National Science Foundation
- EPSCoR [1004094] Funding Source: National Science Foundation
- Office Of The Director [1004094] Funding Source: National Science Foundation
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A study of the two-dimensional crystallization of rhodizonic acid on the crystalline surfaces of gold and copper is presented. Rhodizonic acid, a cyclic oxocarbon related to the ferroelectric croconic acid and the antiferroelectric squaric acid, has not been synthesized in bulk crystalline form yet. Capitalizing on surface-assisted molecular self-assembly, a two-dimensional analogue to the well-known solution-based coordination chemistry, two-dimensional structures of rhodizonic acid were stabilized under ultrahigh vacuum on Au(111) and Cu(111) surfaces. Scanning tunneling microscopy, coupled with first-principles calculations, reveals that on the less reactive Au surface, extended two-dimensional islands of rhodizonic acid are formed, in which the molecules interact via hydrogen bonding and dispersion forces. However, the rhodizonic acid deprotonates into rhodizonate on Cu substrates upon annealing, forming magic clusters and metal-organic coordination networks with substrate adatoms. The networks show a 2:1 distribution of rhodizonate coordinated with 3 and 6 Cu atoms, respectively. The stabilization of crystalline structures of rhodizonic acid, structures not reported before, and their transition into metal organic networks demonstrate the potential of surface chemistry to synthesize new and potential useful organic nanomaterials.
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