4.6 Article

Dynamics at a Janus Interface

期刊

JOURNAL OF PHYSICAL CHEMISTRY C
卷 117, 期 9, 页码 4561-4567

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jp3111259

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资金

  1. National Science Foundation [CHE-1213814]
  2. Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Sciences, U.S. Department of Energy
  3. German Academic Exchange Service
  4. German Science Foundation [KI-768/6-1]
  5. Office of Science of the U.S. Department of Energy [DEAC02-05CH11231]
  6. Extreme Science and Engineering Discovery Environment (XSEDE)
  7. NSF [OCI-1053575]
  8. Division Of Chemistry
  9. Direct For Mathematical & Physical Scien [1213814] Funding Source: National Science Foundation

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Electric field effects on water interfacial properties abound, ranging from electrochemical cells to nanofluidic devices to membrane ion channels. On the nanoscale, spontaneous orientational polarization of water couples with field alignment, resulting in an asymmetric wetting behavior of opposing surfaces-a field-induced analogue of a chemically generated Janus interface. Using atomistic simulations, we uncover a new and significant field polarity (sign) dependence of the dipolarorientation polarization dynamics in the hydration layer. Applying electric fields across a nanoparticle, or a nanopore, can lead to close to 2 orders of magnitude difference in response times of water polarization at opposite surfaces. Typical time scales are within the O(10(-1)) to O(10) picosecond regime. Temporal response to the field change also reveals strong coupling between local polarization and interfacial density relaxations, leading to a nonexponential and in some cases, nonmonotonic response. This work highlights the surprisingly strong asymmetry between reorientational dynamics at surfaces with incoming and which is even more pronounced than the asymmetry in static properties of a field induced Janus interface. outgoing fields,

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