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A major goal of many spectroscopic techniques is to provide comprehensiveinformation on the local chemical environment. Electron transfer mediated decay(ETMD) is a sensitive probe of the environment since it is actively involved inthis non-local radiationless decay process through electron and energy transfersteps. We report the first experimental observation of ETMD in the liquidphase. Using liquid-jet X-ray photoelectron spectroscopy we explore LiClaqueous solution, and detect low-energy electrons unambiguously emerging fromthe ETMD processes of core-ionized Li+. We interpret the experimental resultswith molecular dynamics and high-level ab initio calculations. By consideringvarious solvation-structure models we show that both water molecules and Cl-anions can participate in ETMD, with each process having its characteristicspectral fingerprint. Different ion associations lead to different spectralshapes. The potential application of the unique sensitivity of the ETMDspectroscopy to the local hydration structure and ion pairing is discussed.

First Observation of Electron Transfer Mediated Decay in Aqueous Solutions: A Novel Probe of Ion Pairing