Nature Materials ( IF 37.2 ) Pub Date : 2024-09-24 , DOI: 10.1038/s41563-024-01981-2 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
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.
中文翻译:
涌现的极性超纹理的非平衡途径
超快刺激可以稳定平衡手段无法达到的物质的亚稳态。建立超快激发和亚稳态之间的时空联系对于理解这些现象至关重要。在这里,我们利用单发光泵-X 射线探针测量来捕捉异质结构中出现的持续极性涡旋超晶的快照,该异质结构在设计上具有内置静电和弹性挫折之间的精细平衡。通过用光诱导电荷扰乱这种平衡,在几皮秒内产生极性相位紊乱的最初异质混合物,导致由无序铁电和抑制涡旋序组成的状态。在皮秒-纳秒时间尺度上,瞬态迷宫波动发展,伴随着涡旋序的恢复。在更长的时间尺度上,这些波动逐渐被动态应变调制所抑制,这推动了单个涡旋超晶相的集体出现。我们的结果得到了动力学相场模型的证实,揭示了设计师系统超快激发到持续亚稳态之后的非平衡途径。