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Electrolyte-based transistors utilizing ionic liquids/gels have been highlysuccessful in the study of charge-density-controlled phenomena, particularly inoxides. Experimental probes beyond transport have played a significant role,despite challenges to their application in electric double-layer transistors.Here, we demonstrate application of synchrotron soft X-ray absorptionspectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) as operandoprobes of the charge state and magnetism in ion-gel-gated ferromagneticperovskite films. Electrochemical response via oxygen vacancies at positivegate bias in LaAlO$_3$(001)/La$_{0.5}$Sr$_{0.5}$CoO$_{3-{\delta}}$ is used as atest case. XAS/XMCD measurements of 4-25 unit-cell-thick films first probe theevolution of hole doping (from the O K-edge pre-peak) and ferromagnetism (atthe Co L-edges), to establish a baseline. Operando soft XAS/XMCD ofelectrolyte-gated films is then demonstrated, using optimized spin-coated gelswith thickness $\sim$1 ${\mu}$m, and specific composition. Application of gatevoltages up to +4 V is shown to dramatically suppress the O $K$-edge XASpre-peak intensity and Co $L$-edge XMCD, thus enabling the Co valence andferromagnetism to be tracked upon gate-induced reduction. Soft XAS and XMCD,with appropriate electrolyte design, are thus established as viable for theoperando characterization of electrolyte-gated oxides.

Soft X-ray Absorption Spectroscopy and Magnetic Circular Dichroism as Operando Probes of Complex Oxide Electrolyte Gate Transistors