Non-equilibrium pathways to emergent polar supertextures

Vladimir A Stoica; Tiannan Yang; Sujit Das; Yue Cao; Huaiyu Hugo Wang; Yuya Kubota; Cheng Dai; Hari Padma; Yusuke Sato; Anudeep Mangu; Quynh L Nguyen; Zhan Zhang; Disha Talreja; Marc E Zajac; Donald A Walko; Anthony D DiChiara; Shigeki Owada; Kohei Miyanishi; Kenji Tamasaku; Takahiro Sato; James M Glownia; Vincent Esposito; Silke Nelson; Matthias C Hoffmann; Richard D Schaller; Aaron M Lindenberg; Lane W Martin; Ramamoorthy Ramesh; Iwao Matsuda; Diling Zhu; Long-Q Chen; Haidan Wen; Venkatraman Gopalan; John W Freeland

doi:10.1038/s41563-024-01981-2

Non-equilibrium pathways to emergent polar supertextures

Nat Mater. 2024 Oct;23(10):1394-1401. doi: 10.1038/s41563-024-01981-2. Epub 2024 Sep 24.

Authors

Vladimir A Stoica^#^{1

2}, Tiannan Yang^#^{3

4}, Sujit Das^#⁵, Yue Cao⁶, Huaiyu Hugo Wang³, Yuya Kubota^{7

8}, Cheng Dai³, Hari Padma³, Yusuke Sato⁹, Anudeep Mangu¹⁰, Quynh L Nguyen^{11

12}, Zhan Zhang¹³, Disha Talreja³, Marc E Zajac¹³, Donald A Walko¹³, Anthony D DiChiara¹³, Shigeki Owada^{7

8}, Kohei Miyanishi⁸, Kenji Tamasaku^{7

8}, Takahiro Sato¹¹, James M Glownia¹¹, Vincent Esposito¹¹, Silke Nelson¹¹, Matthias C Hoffmann¹¹, Richard D Schaller¹⁴, Aaron M Lindenberg^{10

12

15}, Lane W Martin^{16

17

18}, Ramamoorthy Ramesh^{16

17

18}, Iwao Matsuda⁹, Diling Zhu¹¹, Long-Q Chen³, Haidan Wen^{19

20}, Venkatraman Gopalan²¹, John W Freeland²²

Affiliations

¹ Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA, USA. [email protected].
² Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA. [email protected].
³ Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA, USA.
⁴ Interdisciplinary Research Centre, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai, China.
⁵ Materials Research Centre, Indian Institute of Science, Bangalore, India.
⁶ Materials Science Division, Argonne National Laboratory, Lemont, IL, USA.
⁷ Japan Synchrotron Radiation Research Institute, Sayo, Japan.
⁸ RIKEN SPring-8 Center, Sayo, Japan.
⁹ Institute for Solid State Physics, The University of Tokyo, Kashiwa, Japan.
¹⁰ Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA.
¹¹ Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
¹² Stanford PULSE Institute, SLAC National Accelerator Laboratory & Stanford University, Menlo Park, CA, USA.
¹³ Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA.
¹⁴ Center for Nanoscale Materials, Argonne National Laboratory, Lemont, IL, USA.
¹⁵ Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
¹⁶ Department of Materials Science and Engineering & Department of Physics, University of California, Berkeley, CA, USA.
¹⁷ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
¹⁸ Rice University, Houston, TX, USA.
¹⁹ Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA. [email protected].
²⁰ Materials Science Division, Argonne National Laboratory, Lemont, IL, USA. [email protected].
²¹ Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA, USA. [email protected].
²² Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA. [email protected].

^# Contributed equally.

PMID: 39317816
DOI: 10.1038/s41563-024-01981-2

Abstract

Ultrafast stimuli can stabilize metastable states of matter inaccessible by equilibrium means. Establishing the spatiotemporal link between ultrafast excitation and metastability is crucial to understand these phenomena. Here we utilize single-shot optical pump-X-ray probe measurements to capture snapshots of the emergence of a persistent polar vortex supercrystal in a heterostructure that hosts a fine balance between built-in electrostatic and elastic frustrations by design. By perturbing this balance with photoinduced charges, an initially heterogeneous mixture of polar phase disorders within a few picoseconds, leading to a state composed of disordered ferroelectric and suppressed vortex orders. On the picosecond-nanosecond timescales, transient labyrinthine fluctuations develop, accompanied by the recovery of the vortex order. On longer timescales, these fluctuations are progressively quenched by dynamical strain modulations, which drive the collective emergence of a single vortex supercrystal phase. Our results, corroborated by dynamical phase-field modelling, reveal non-equilibrium pathways following the ultrafast excitation of designer systems to persistent metastability.

Abstract

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