Journal
LANGMUIR
Volume 31, Issue 24, Pages 6924-6932Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.langmuir.5b01498
Keywords
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Funding
- Robert A. Welch Foundation [F-1464]
- National Science Foundation [CBET-140378]
- NSF
- NIH/NIGMS via NSF [DMR-0936384]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1403768] Funding Source: National Science Foundation
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Dodecanethiol-capped gold (Au) nanocrystal superlattices can undergo a surprisingly diverse series of ordered structure transitions when heated (Goodfellow, B. W.; Rasch, M. R; Hessel, C. M.; Patel, R. N.; Smilgies, D.-M.; Korgel, B. A. Nano Lett. 2013, 13, 5710-5714). These are the result of highly uniform changes in nanocrystal size, which subsequently force a spontaneous rearrangement of superlattice structure. Here, we show that halide-containing surfactants play an essential role in these transitions. In the absence of any halide-containing surfactant, superlattices of dodecanethiol-capped (1.9-nm-diameter) Au nanocrystals do not change size until reaching about 190-205 degrees C, at which point the gold cores coalesce. In the presence of halide-containing surfactant, such as tetraoctylphosphonium bromide (TOPB) or tetraoctylammounium bromide (TOAB), the nanocrystals ripen at much lower temperature and superlattices undergo various ordered structure transitions upon heating. Chloride- and iodide-containing surfactants induce similar behavior, destabilizing the Au thiol bond and reducing the thermal stability of the nanocrystals.
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