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DOE OSTI · 3365441

Photoinduced correlations in stochastic dynamics of a solid-state ionic conductor

McClellan, Jackson [University of California, Berkeley, CA (United States); The Ohio State Univ., Columbus, OH (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division]·Zong, Alfred [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division; Stanford Univ., CA (United States)] (ORCID:0000000320473801)·Pham, Kim H. [California Institute of Technology (CalTech), Pasadena, CA (United States)]·Liu, Hanzhe [California Institute of Technology (CalTech), Pasadena, CA (United States); Purdue Univ., West Lafayette, IN (United States)]·Iton, Zachery W. B. [California Institute of Technology (CalTech), Pasadena, CA (United States)]·Guzelturk, Burak [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:0000000319776485)·Walko, Donald A. [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:0009000163749575)·Wen, Haidan [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Argonne National Laboratory (ANL), Argonne, IL (United States). Materials Science Division] (ORCID:000000025427175X)·Cushing, Scott K. [California Institute of Technology (CalTech), Pasadena, CA (United States)]·Zuerch, Michael W. [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division] (ORCID:0000000151512119)
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Abstract

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and probing complex molecular dynamics. The photoresponse following a laser pulse is generally nonidentical between exposures due to spatiotemporal fluctuations or the stochastic nature of dynamical pathways. However, most ultrafast pump-probe experiments struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing deviations from the averaged response. Leveraging the stability and high photon flux of time-resolved X-ray micro-diffraction at a synchrotron, we characterized stochastic photoinduced dynamics in a solid-state ionic conductor. By analyzing temporal evolutions of the lattice parameter of a single grain, we found that shot-to-shot fluctuations are not independent. Instead, correlations exist between nonequilibrium lattice trajectories following adjacent shots, with a characteristic correlation length of approximately 1500 shots, corresponding to an energy barrier of 0.4 ± 0.1 eV, close to the activation energy of lithium-ion diffusion.

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36 MATERIALS SCIENCE37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

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McClellan, Jackson [University of California, Berkeley, CA (United States); The Ohio State Univ., Columbus, OH (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division], Zong, Alfred [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division; Stanford Univ., CA (United States)] (ORCID:0000000320473801), Pham, Kim H. [California Institute of Technology (CalTech), Pasadena, CA (United States)], Liu, Hanzhe [California Institute of Technology (CalTech), Pasadena, CA (United States); Purdue Univ., West Lafayette, IN (United States)], Iton, Zachery W. B. [California Institute of Technology (CalTech), Pasadena, CA (United States)], Guzelturk, Burak [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:0000000319776485), Walko, Donald A. [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:0009000163749575), Wen, Haidan [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Argonne National Laboratory (ANL), Argonne, IL (United States). Materials Science Division] (ORCID:000000025427175X), Cushing, Scott K. [California Institute of Technology (CalTech), Pasadena, CA (United States)], Zuerch, Michael W. [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Materials Sciences Division] (ORCID:0000000151512119). 2026-05-15. Photoinduced correlations in stochastic dynamics of a solid-state ionic conductor. https://doi.org/10.1038/s41467-026-72663-7

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