Emergent Higher-Order Optical Nonlinearity in Self-Assembled Polar Supertextures
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.
Authors
- Peter Benjamin Meisenheimer (ORCID: https://orcid.org/0000-0002-8903-3065)
- Venkatraman Gopalan (ORCID: https://orcid.org/0000-0001-6866-3677)
- Aiden Ross (ORCID: https://orcid.org/0009-0001-8195-6172)
- W. Z. Hu (ORCID: https://orcid.org/0000-0002-0926-0760)
- Sujit Das (ORCID: https://orcid.org/0000-0001-9823-0207)
- Daniel Alejandro Bustamante Lopez (ORCID: https://orcid.org/0000-0003-0012-6335)
- Akash Surampalli (ORCID: https://orcid.org/0009-0007-7857-357X)
- Lane W. Martin (ORCID: https://orcid.org/0000-0003-1889-2513)
- Vladimir Alexandru Stoica (ORCID: https://orcid.org/0000-0002-2734-7819)
- Xianghan Xu (ORCID: https://orcid.org/0000-0001-6854-300X)
- Deepankar Sri Gyan (ORCID: https://orcid.org/0000-0003-1672-2617)
- Sang‐Wook Cheong (ORCID: https://orcid.org/0000-0001-9905-6175)
- Long‐Qing Chen (ORCID: https://orcid.org/0000-0003-3359-3781)
- Mohit Tanwani (ORCID: https://orcid.org/0009-0001-4534-9244)
- Ramamoorthy Ramesh
- Xiaojiang Li
Institutions
- Rutgers, The State University of New Jersey (US)
- Boston University (US)
- Pennsylvania State University (US)
- Lawrence Berkeley National Laboratory (US)
- St. Mary's University, Texas (US)
- University of California System (US)
- Rutgers Sexual and Reproductive Health and Rights (NL)
- Indian Institute of Science Bangalore (IN)
- Rice University (US)
- University of California, Berkeley (US)
Publication Details
- Journal
- ACS Nano
- Published
- 2026-10-26
- DOI
- https://doi.org/10.1021/acsnano.6c10644
- Primary Topic
- Photorefractive and Nonlinear Optics
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Indian Institute of Science
- Ministry of Education, India
- Basic Energy Sciences
- Army Research Office
- National Science Foundation Graduate Research Fellowship Program