Papers › Correlated Terahertz phonon-ion interactions control ion conduction in a solid electrolyte
Correlated Terahertz phonon-ion interactions control ion conduction in a solid electrolyte
Kim H. Pham, Kiarash Gordiz, Natan A. Spear, Amy K. Lin, Jonathan M. Michelsen, Hanzhe Liu, Daniele Vivona, Geoffrey A. Blake, Yang Shao-Horn, Asegun Henry, Kimberly A. See, Scott K. Cushing
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Ionic conduction in solids that exceeds 1 mS/cm is predicted to involve coupled phonon-ion interactions in the crystal lattice. Here, we use theory and experiment to measure the possible contribution of coupled phonon-ion hopping modes which enhance Li+ migration in Li0.5La0.5TiO3 (LLTO). The ab initio calculations predict that the targeted excitation of individual TiO6 rocking modes greatly increases the Li+ jump rate as compared to the excitation of vibrational modes associated with heating. Experimentally, coherently driving TiO6 rocking modes via terahertz (THz) illumination leads to a ten-fold decrease in the differential impedance compared to the excitation of acoustic and optical phonons. Additionally, we differentiate the ultrafast responses of LLTO due to ultrafast heating and THz-range vibrations using laser-driven spectroscopy (LUIS), finding a unique long-lived response for the THz-range excitation. These findings provide new insights into coupled ion migration mechanisms, indicating the important role of THz-range coupled phonon-ion hopping modes in enabling fast ion conduction at room temperature.
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