Correlated Terahertz phonon-ion interactions control ion conduction in a solid electrolyte
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arXiv
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| Format: | Preprint |
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2023
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| _version_ | 1866914219223416832 |
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| author | Pham, Kim H. Gordiz, Kiarash Spear, Natan A. Lin, Amy K. Michelsen, Jonathan M. Liu, Hanzhe Vivona, Daniele Blake, Geoffrey A. Shao-Horn, Yang Henry, Asegun See, Kimberly A. Cushing, Scott K. |
| author_facet | Pham, Kim H. Gordiz, Kiarash Spear, Natan A. Lin, Amy K. Michelsen, Jonathan M. Liu, Hanzhe Vivona, Daniele Blake, Geoffrey A. Shao-Horn, Yang Henry, Asegun See, Kimberly A. Cushing, Scott K. |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2305_01632 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Correlated Terahertz phonon-ion interactions control ion conduction in a solid electrolyte Pham, Kim H. Gordiz, Kiarash Spear, Natan A. Lin, Amy K. Michelsen, Jonathan M. Liu, Hanzhe Vivona, Daniele Blake, Geoffrey A. Shao-Horn, Yang Henry, Asegun See, Kimberly A. Cushing, Scott K. Materials Science Chemical Physics 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. |
| title | Correlated Terahertz phonon-ion interactions control ion conduction in a solid electrolyte |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2305.01632 |