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Superionic conductors, or solid-state ion-conductors that surpass 0.01 S/cmin conductivity, can enable more energy dense batteries, robust artificial ionpumps, and optimized fuel cells. However, tailoring superionic conductorsrequire precise knowledge of ion migration mechanisms that are still not wellunderstood, due to limitations set by available spectroscopic tools. Mostspectroscopic techniques do not probe ion hopping on its inherent picosecondtimescale, nor the many-body correlations between the migrating ions, latticevibrational modes, and charge screening clouds--all of which are posited togreatly enhance ionic conduction. Here, we develop an ultrafast technique thatmeasures the time-resolved change in impedance upon light excitation whichtriggers selective ion-coupled correlations. We apply our proposed technique tostudy a solid-state Li+ conductor Li0.5La0.5TiO3 (LLTO). We compare therelative change in impedance of LLTO before and after a UV to THz frequencyexcitation to map the corresponding ion-many-body-interaction correlations. Wealso develop a cost-effective, non-time-resolved laser-driven impedance methodthat is more accessible for lab-scale adoption. From both our techniques, wedetermine that electronic screening and phonon-mode interactions dominate theion migration pathway of LLTO. Although we only present one case study, ourtechnique can also probe O2-, H+, or other ion and charge carrier transportphenomena where ultrafast correlations control transport. Furthermore, thetemporal relaxation of the measured impedance can distinguish ion transporteffects caused by many-body correlations, optical heating, correlation, andmemory behavior.

Laser-driven ultrafast impedance spectroscopy for measuring complex ion hopping processes