1：Experimental Design and Method Selection:

The study employs a combination of methods including thermal analysis, dielectric and electric studies, optical observations, EPR and 1H NMR spectroscopy, and quasielastic neutron scattering (QENS) to analyze molecular motion and phase transitions.

2：Sample Selection and Data Sources:

Single crystals of MAFe, DMAFe, and TrMAFe were prepared by reacting methyl-, dimethyl-, trimethylamine hydrochloride with K3Fe(CN)6 in a molar ratio of 3:1, recrystallized from deionized water, and confirmed by elemental analysis.

3：List of Experimental Equipment and Materials:

Instruments include PerkinElmer DSC 8500 calorimeter, Setaram SETSYS 16/18 for TGA/DTA, Bruker ELEXSYS E580 EPR spectrometer, Agilent E4980A LCR Meter, HP 4191A impedance analyzer, Keithley 6517D electrometer, Aixact equipment for polarization, Trek 609E6 voltage amplifier, Olympus BX53 microscope with LINKAM THM-600 stage, SPHERES neutron spectrometer, ELLAB TEL-Atomic PS 15 NMR spectrometer, and UNIPAN 660 temperature controller. Materials include methyl-, dimethyl-, trimethylamine hydrochloride (Sigma, ≥98%), K3Fe(CN)6 (Sigma-Aldrich, ≥99.0%), deionized water, silver conductive paint (Electron Microscopy Sciences, 503).

4：0%), deionized water, silver conductive paint (Electron Microscopy Sciences, 503). Experimental Procedures and Operational Workflow:

4. Experimental Procedures and Operational Workflow: Crystals were synthesized, characterized, and subjected to various measurements across temperature ranges (e.g., 100-360 K for DSC, 150-500 K for dielectric, 100-300 K for QENS). Specific procedures include cooling/heating cycles, application of electric fields, and data collection at multiple frequencies and temperatures.

5：Data Analysis Methods:

Data were analyzed using software like SLAW and FRIDA for neutron data, Arrhenius plots for conductivity, fitting models for QENS and NMR data, and numerical integration for second moments.