Journal
PHYSICAL REVIEW LETTERS
Volume 108, Issue 5, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.108.055502
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Funding
- National Research Foundation (NRF)
- Korea government (MEST) [2011-0017435]
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-AC02-07CH11358]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- KAKENHI by MEXT, Japan [23350005)]
- Grants-in-Aid for Scientific Research [23350005, 19105005] Funding Source: KAKEN
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Surface crystallization at the vapor-liquid interface of the ionic liquid (1-butyl-3-methylimidazolium hexafluorophosphate) is observed in synchrotron x-ray diffraction studies. Sharp Bragg reflections emerge in grazing-angle x-ray diffraction patterns 37 degrees C above the bulk melting temperature, indicating the presence of a long-range ordered phase at the surface in coexistence with the bulk parent liquid. The unique structure of the vapor-liquid interface where butyl chains attached to the cations are expelled to the vapor side facilitates interionic electrostatic interactions that lead to the crystallization. Our results demonstrate the complexity of ionic-liquid structure with their tendency to spontaneously phase separate into nanodomains with finite correlation lengths in coexistence with the liquid phase. By virtue of interfacial boundary conditions, these nanodomains grow laterally to form quasi-two-dimensional crystals.
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