Journal
PHYSICAL REVIEW LETTERS
Volume 125, Issue 11, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.125.116001
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Funding
- MIT-Imperial College Seed Fund
- Center for Enhanced Nanofluidic Transport, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0019112]
- National Science Foundation Graduate Research Fellowship [1122374]
- Amar G. Bose Research Grant
- Centre for Doctoral Training on Theory and Simulation of Materials at Imperial College London - EPSRC [EP/L015579/1]
- Thomas Young Centre [TYC-101]
- The Leverhulme Trust [RPG2016-223]
- EPSRC [EP/H004319/1] Funding Source: UKRI
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Ions in ionic liquids and concentrated electrolytes reside in a crowded, strongly interacting environment, leading to the formation of discrete layers of charges at interfaces and spin-glass structure in the bulk. Here, we propose a simple theory that captures the coupling between steric and electrostatic forces in ionic liquids. The theory predicts the formation of discrete layers of charge at charged interfaces. Further from the interface, or at low polarization of the electrode, the model outputs slowly decaying oscillations in the charge density with a wavelength of a single ion diameter, as shown by analysis of the gradient expansion. The gradient expansion suggests a new structure for partial differential equations describing the electrostatic potential at charged interfaces. We find quantitative agreement between the theory and molecular simulations in the differential capacitance and concentration profiles.
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