DOE OSTI · 3374708
Decoding THz‐Driven Dynamic Fingerprints of Ferroelectric Nanotwin Networks
Abstract
Ultrafast polarization dynamics in ferroelectrics are of considerable interest for high-speed tunable dielectrics and electro-optics. Extended domain wall networks formed in ferroelectric twin nanodomains can support collective dynamics in the terahertz regime but require techniques that track polarization and strain evolution driven by ultrafast stimulus. Here, we use multi-modal probing of THz-pulse-driven excitations in PbTiO 3 /SrTiO 3 superlattices by combining X-ray free electron laser measurements that directly tracks lattice changes, with optical second harmonic generation that tracks the electronic potential coupled with the lattice potential. Dynamical phase-field modeling enables fingerprinting of these collective modes as superpositions of domain “breathing” through wall oscillations and polarization “rotations” with still walls. Ultrafast domain wall motion at 0.1–0.5 THz is observed at practical fields of 100 kV/cm with wall velocities of >4000 m/s, approaching typical speed of sound in PbTiO 3 . A unique “charging” mode is discovered that can electrically charge and discharge domain walls on ∼4 ps time scale thus dynamically tuning wall conductivity. Integrated experimental and theoretical fingerprinting of the dynamical landscape presented here enables ultrafast control of ferroics for high-speed microelectronics and optical applications.
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Li, Xiaojiang [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000315356109), Ross, Aiden [Pennsylvania State University, University Park, PA (United States)] (ORCID:0009000181956172), Stoica, Vladimir A. [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000227347819), Das, Sujit [Indian Institute of Science, Bangalore (India)] (ORCID:0000000198230207), Hazra, Sankalpa [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000291268058), Wang, Huaiyu (Hugo) [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000175551198), Padma, Hari [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000306821849), Hoffmann, Matthias C. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000235969853), Kramer, Patrick [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000185891540), Song, Sanghoon [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000334931850), Nelson, Silke [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000229376074), Sato, Takahiro [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000322020910), Zhu, Diling [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0009000149419799), Ramesh, Ramamoorthy [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000305241332), Martin, Lane W. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Rice University, Houston, TX (United States)] (ORCID:0000000318892513), Cao, Yue [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:000000023989158X), Freeland, John W. [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000348145308), Lindenberg, Aaron M. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford University, CA (United States)] (ORCID:0000000332337161), Wen, Haidan [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:000000025427175X), Chen, Long‐Qing [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000333593781), Gopalan, Venkatraman [Pennsylvania State University, University Park, PA (United States)] (ORCID:0000000168663677). 2026-05-02. Decoding THz‐Driven Dynamic Fingerprints of Ferroelectric Nanotwin Networks. https://doi.org/10.1002/adma.73118
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