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PreprintCC BY 4.0arXiv

Emergent higher-order optical nonlinearity in self-assembled polar supertextures

  • Daniel A. Bustamante Lopez
  • Deepankar Sri Gyan
  • Xiaojiang Li
  • Vladimir A. Stoica
  • Sujit Das
  • Peter Meisenheimer
  • Akash Surampalli
  • Mohit Tanwani
  • Xianghan Xu
  • Aiden Ross
  • Long-Qing Chen
  • Sang-Wook Cheong
4 more authors
  • Lane W. Martin
  • Ramamoorthy Ramesh
  • Venkatraman Gopalan
  • Wanzheng Hu
Open at sourcePDFDOICite

Abstract

Giant optical nonlinearities enable advanced materials control and bridge exotic light-matter phenomena to next-generation photonics. However, materials exhibiting strong higher-order optical nonlinearity beyond the second order are typically rare. Here, we report the discovery of a giant and ultrafast second-harmonic generation (SHG) in self-assembled polar skyrmions under mid-infrared excitations. The transient SHG intensity exhibits a distinctive power dependence originating from higher-order nonlinearity. More generally, we show that large higher-order nonlinearity emerges across diverse domain structures in polar superlattices. Phase-field simulations demonstrate a strong and periodic local permittivity variation within each polar texture at equilibrium, and further confirm the fast polarization oscillation in polar skyrmions with mid-infrared excitations. This intense local permittivity modulation can satisfy epsilon-near-zero conditions, unlocking dramatically enhanced nonlinear optical responses without photonic engineering. Consequently, the self-assembled polar topologies with strong inherent optical nonlinearity could establish a platform for quantum information processing and high-speed optical communications.

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Cite

BibTeXRIS
BibTeX
@misc{lopez2026emergent,
  title = {{Emergent higher-order optical nonlinearity in self-assembled polar supertextures}},
  author = {Daniel A. Bustamante Lopez and Deepankar Sri Gyan and Xiaojiang Li and Vladimir A. Stoica and Sujit Das and Peter Meisenheimer and Akash Surampalli and Mohit Tanwani and Xianghan Xu and Aiden Ross and Long-Qing Chen and Sang-Wook Cheong and Lane W. Martin and Ramamoorthy Ramesh and Venkatraman Gopalan and Wanzheng Hu},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.38138},
  eprint = {2610.38138},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.38138},
  note = {CC BY 4.0},
}
RIS
TY  - UNPB
TI  - Emergent higher-order optical nonlinearity in self-assembled polar supertextures
AU  - Daniel A. Bustamante Lopez
AU  - Deepankar Sri Gyan
AU  - Xiaojiang Li
AU  - Vladimir A. Stoica
AU  - Sujit Das
AU  - Peter Meisenheimer
AU  - Akash Surampalli
AU  - Mohit Tanwani
AU  - Xianghan Xu
AU  - Aiden Ross
AU  - Long-Qing Chen
AU  - Sang-Wook Cheong
AU  - Lane W. Martin
AU  - Ramamoorthy Ramesh
AU  - Venkatraman Gopalan
AU  - Wanzheng Hu
PY  - 2026
DA  - 2026/10/28
PB  - arXiv
DO  - 10.48550/arxiv.2610.38138
UR  - https://arxiv.org/abs/2610.38138
AB  - Giant optical nonlinearities enable advanced materials control and bridge exotic light-matter phenomena to next-generation photonics. However, materials exhibiting strong higher-order optical nonlinearity beyond the second order are typically rare. Here, we report the discovery of a giant and ultrafast second-harmonic generation (SHG) in self-assembled polar skyrmions under mid-infrared excitations. The transient SHG intensity exhibits a distinctive power dependence originating from higher-order nonlinearity. More generally, we show that large higher-order nonlinearity emerges across diverse domain structures in polar superlattices. Phase-field simulations demonstrate a strong and periodic local permittivity variation within each polar texture at equilibrium, and further confirm the fast polarization oscillation in polar skyrmions with mid-infrared excitations. This intense local permittivity modulation can satisfy epsilon-near-zero conditions, unlocking dramatically enhanced nonlinear optical responses without photonic engineering. Consequently, the self-assembled polar topologies with strong inherent optical nonlinearity could establish a platform for quantum information processing and high-speed optical communications.
ER  -