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Ferrorotational domain walls revealed by electric quadrupole second harmonic generation microscopy

Xiaoyu Guo1, Rachel Owen1, Austin Kaczmarek1, Xiaochen Fang2, Chandan De3,4,5, Youngjun Ahn1, Wei Hu6,7, Nishkarsh Agarwal8, Suk Hyun Sung8 et al.

Robert Hovden8, Sang-Wook Cheong2, and Liuyan Zhao1,*

  • 1Department of Physics, University of Michigan, Ann Arbor, Michigan 48109, USA
  • 2Department of Physics and Astronomy, Rutgers Center for Emergent Materials, Rutgers University, Piscataway, New Jersey 08854, USA
  • 3Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science (IBS), Pohang 37673, Korea
  • 4Laboratory of Pohang Emergent Materials, Pohang Accelerator Laboratory, Pohang 37673, Korea
  • 52D Crystal Consortium, Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, USA
  • 6School for Environment and Sustainability, University of Michigan, Ann Arbor, Michigan 48109, USA
  • 7Department of Statistics, University of Michigan, Ann Arbor, Michigan 48109, USA
  • 8Department of Material Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA

  • *Corresponding author: lyzhao@umich.edu

Phys. Rev. B 107, L180102 – Published 24 May, 2023

DOI: https://doi.org/10.1103/PhysRevB.107.L180102

Abstract

Domain walls are ubiquitous in materials that undergo phase transitions driven by spontaneous symmetry breaking. Domain walls in ferroics and multiferroics have received tremendous attention recently due to their emergent properties distinct from their domain counterparts—for example, their high mobility and controllability, as well as their potential applications in nanoelectronics. However, it is extremely challenging to detect, visualize, and study the ferrorotational (FR) domain walls because the FR order, in contrast to ferromagnetism and ferroelectricity, is invariant under both the spatial-inversion and the time-reversal operations and, thus, hardly couple with conventional experimental probes. Here, a FR candidate NiTiO3 is investigated by ultrasensitive electric quadrupole (EQ) second-harmonic generation rotational anisotropy (SHG RA) to probe the point symmetries of the two degenerate FR domain states, showing their relation by the vertical mirror operations that are broken below the FR critical temperature. We then visualize the real-space FR domains by scanning EQ SHG microscopy, and further, resolve the FR domain walls by revealing a suppressed SHG intensity at the domain walls. By taking local EQ SHG RA measurements, we show the restoration of the mirror symmetry at FR domain walls and prove their unconventional nonpolar nature. Our findings not only provide a comprehensive insight into FR domain walls, but also demonstrate a unique and powerful tool for future studies on domain walls of unconventional ferroics both of which pave the way towards future manipulations and applications of FR domain walls.

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