DOE OSTI · 3012959
Hidden domain boundary dynamics toward crystalline perfection
Abstract
A central paradigm of nonequilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex mesoscopic systems requires probing the microscopic trajectories associated with irreversible processes, the role of fluctuations and entropy growth, and the timescales on which nonequilibrium responses are ultimately maintained. Approaches that illuminate these processes in model systems may enable a more general understanding of other heterogeneous nonequilibrium phenomena, and potentially define ultimate speed and energy cost limits for information processing technologies. Here, we apply ultrafast single-shot X-ray photon correlation spectroscopy to resolve the nonequilibrium, heterogeneous, and irreversible mesoscale dynamics during a light-induced phase transition in a (PbTiO 3 ) 16 /(SrTiO 3 ) 16 superlattice. Such ferroelectric superlattice systems are a useful platform to study phase transitions and topological dynamics due to their high degree of tunability. This provides an approach for capturing the nucleation of the light-induced phase, the formation of transient mesoscale defects at the boundaries of the nuclei, and the eventual annihilation of these defects, even in systems with complex polarization topologies. We identify a nonequilibrium correlation response spanning >10 orders of magnitude in timescales, with multistep behavior similar to the plateaus observed in supercooled liquids and glasses. We further show how the observed time-dependent long-time correlations can be understood in terms of stochastic and non-Markovian dynamics of domain walls, encoded in waiting-time distributions with power-law tails. This work defines possibilities for probing the nonequilibrium and correlated dynamics of disordered and heterogeneous media.
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Mangu, Anudeep [Stanford University, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000255968348), Stoica, Vladimir A. [Pennsylvania State University, University Park, PA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:0000000227347819), Zheng, Hao [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Yang, Tiannan [Pennsylvania State Univ., University Park, PA (United States)], Zhang, Maohua [Pennsylvania State Univ., University Park, PA (United States)], Wang, Huaiyu (Hugo) [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000175551198), Zu, Rui [Pennsylvania State Univ., University Park, PA (United States)], Nguyen, Quynh L. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)], Song, Sanghoon [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)], Das, Sujit [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States); Indian Institute of Science, Bangalore (India)] (ORCID:0000000198230207), Meisenheimer, Peter [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)], Donoway, Elizabeth [University of California, Berkeley, CA (United States)] (ORCID:0000000253496682), Chollet, Matthieu [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)], Sun, Yanwen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)] (ORCID:0000000159266565), Turner, Joshua J. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)] (ORCID:0000000221067955), Freeland, John W. [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Wen, Haidan [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)] (ORCID:000000025427175X), Martin, Lane W. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States); Rice University, Houston, TX (United States)], Chen, Long-Qing [Pennsylvania State Univ., University Park, PA (United States)], Gopalan, Venkatraman [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000168663677), Zhu, Diling [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)], Cao, Yue [Argonne National Laboratory (ANL), Argonne, IL (United States)], Lindenberg, Aaron M. [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE)] (ORCID:0000000332337161). 2025-01-08. Hidden domain boundary dynamics toward crystalline perfection. https://doi.org/10.1073/pnas.2407772122
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