Configurational evidence for antiferromagnetic interaction in disordered magnetic ionic liquids by X-ray scattering-aided hybrid reverse Monte Carlo simulation

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Fig. 1. Corrected X-ray scattering profiles of Emim[FeCl4] (top) and Bmim[FeCl4]

(bottom). The dashed curves indicate the sum of the independent atomic scattering

profiles of each IL. Vertical blue dashed lines indicate the peak positions of Emim[FeCl4]

provided to guide the eye.

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Fig. 2. (a,b) Electron radial functions (ERDFs) of (a) Emim[FeCl4] and (a) Bmim[FeCl4].

Open circles and solid lines denote the experimental results and the results of the HRMC

simulations, respectively. (c,d) Each component ERDF obtained by HRMC simulations

for (c) Emim[FeCl4] and (d) Bmim[FeCl4], with intra-molecule (sky blue), inter anion

(green), inter cation-anion (blue), and inter cation (red) components shown.

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Fig. 3. Spatial distribution functions (SDFs) of Emim[FeCl4] (top) and Bmim[FeCl4]

(bottom) for the 1st coordination structure of Fe around the cations evaluated by HRMC

simulations. In these figures, the plane of the imidazolium ring is parallel to the x-y plane

and the z direction is perpendicular to the x-y plane. Cyan, blue, and white spheres

represent carbon, nitrogen, and hydrogen atoms, respectively.

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Fig. 4. (a) Temperature dependence of the X-ray scattering profiles of Bmim[FeCl4] from

90 K to 523 K. (b) ERDFs of Bmim[FeCl4] at 90 K (red), 298 K (green), and 523 K

(purple). (c) Component anion-anion ERDFs evaluated by HRMC simulations for

Bmim[FeCl4] at 90 K (red), 298 K (green), and 523 K (purple). Inset shows the SDF of

the nearest Cl atoms around the FeCl4 ion at 90 K. Here, green and gray spheres represent

the chlorine and iron atoms of the FeCl4 ion, respectively.

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Fig. 5. Spatial distribution functions of Bmim[FeCl4] for the 1st coordination structure

of Fe around the cations evaluated using HRMC simulations at 90 K (left), 298 K (center),

and 523 K (right). In these figures, the plane of the imidazolium ring is parallel to the x-

y plane, and the z direction is perpendicular to the x-y plane.

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Fig. 6. Distribution of the assembling number of neighboring FeCl4- ions in

Bmim[FeCl4] at 90 K. Here, we defined the Cl-Cl neighbor distance as less than 0.39 nm.

(Inset) 3-, 4-, 5-, and 6-member networks of FeCl4- ions in the simulation snapshot. Green

and gray spheres represent the Cl and Fe atoms, respectively. Red lines connect the Fe

atoms in the Fe-Cl-Cl-Fe networks.

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