Nonresonant Raman Control of Ferroelectric Polarization
Important advances is recently made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes is experimentally observed and proposed for dynamic material control, but the resulting atomic excursion is limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.
Authors
- David A. Reis (ORCID: https://orcid.org/0000-0002-1576-7533)
- Christian Heide (ORCID: https://orcid.org/0000-0002-7652-3241)
- Yuejun Shen
- Keith A. Nelson (ORCID: https://orcid.org/0000-0001-7804-5418)
- Jiaojian Shi (ORCID: https://orcid.org/0009-0000-2770-7784)
- Shambhu Ghimire (ORCID: https://orcid.org/0000-0002-0260-951X)
- Haowei Xu (ORCID: https://orcid.org/0000-0002-5360-5738)
- Aaron M. Lindenberg (ORCID: https://orcid.org/0000-0003-3233-7161)
- Edoardo Baldini (ORCID: https://orcid.org/0000-0002-8131-9974)
- Tony F. Heinz (ORCID: https://orcid.org/0000-0003-1365-9464)
- Meredith Henstridge (ORCID: https://orcid.org/0000-0002-7561-0802)
- Anudeep Mangu (ORCID: https://orcid.org/0000-0002-5596-8348)
- Ju Li (ORCID: https://orcid.org/0000-0002-7841-8058)
- Jian Zhou (ORCID: https://orcid.org/0000-0002-2606-4833)
- Mariano Trigo
- Xinyue Peng (ORCID: https://orcid.org/0000-0002-7352-7554)
- Shangjie Zhang
- Isabel Sedwick
Institutions
- University of Washington (US)
- SLAC National Accelerator Laboratory (US)
- Stanford Health Care (US)
- Massachusetts Institute of Technology (US)
- The University of Texas at Austin (US)
- Xi'an Jiaotong University (CN)
- Stanford University (US)
Publication Details
- Journal
- Advanced Materials
- Published
- 2025-08-25
- DOI
- https://doi.org/10.1002/adma.202510524
- Primary Topic
- Photorefractive and Nonlinear Optics
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Science Foundation
- U.S. Department of Energy
- University of Washington
- National Natural Science Foundation of China
- Multidisciplinary University Research Initiative
- Air Force Office of Scientific Research