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The recent boom of energy storage and conversion devices, exploiting ionic liquids (ILs) to enhance the performance, requires an in-depth understanding of this new class of electrolytes in device operation conditions. One central question critical to device performance is how the mobile ions accumulate near charged electrodes. Here, we present the excess ion depth profiles of ILs in ionomer membrane actuators (Aquivion/1-butyl-2,3-dimethylimidazolium chloride (BMMI-Cl), 27 μm thick), characterized directly by Time-of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS) at liquid nitrogen temperature. Experimental results reveal that for the IL studied, cations and anions are accumulated at both electrodes. The large difference in the total volume occupied by the excess ions between the two electrodes cause the observed large bending actuation of the actuator. Hence we demonstrate that ToF-SIMS experiment provides great insights on the physics nature of ionic devices.

An organic delta layer system made of alternating Langmuir Blodgett multilayers of barium arachidate (AA) and barium dimyristoyl phosphatidate (DMPA) was constructed to elucidate the factors that control depth resolution in molecular depth profile experiments. More specifically, one or several bilayers of DMPA (4.4 nm) were embedded in relatively thick (51 to 105 nm) multilayer stacks of AA, resulting in a well-defined delta-layer model system closely resembling a biological membrane. 3-D imaging ToF-SIMS depth profile analysis was performed on this system using a focused buckminsterfullerene (C60) cluster ion beam. The delta layer depth response function measured in these experiments exhibits similar features as those determined in inorganic depth profiling, namely an asymmetric shape with quasi-exponential leading and trailing edges and a central Gaussian peak. The effects of sample temperature, primary ion kinetic energy and incident angle on the depth resolution were investigated. While the information depth of the acquired SIMS spectra was found to be temperature independent, the depth resolution was found to be significantly improved at low temperature. Ion induced mixing is proposed to be largely responsible for the broadening, rather than topography, as determined by AFM, therefore depth resolution can be optimized using lower kinetic energy, glancing angle and liquid nitrogen temperature.

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