Nonresonant Raman Control of Ferroelectric Polarization

Jiaojian Shi^{1

2

3}, Christian Heide^{4

5}, Haowei Xu⁶, Yuejun Shen¹, Meredith Henstridge⁷, Isabel Sedwick³, Anudeep Mangu¹, Xinyue Peng⁸, Shangjie Zhang⁸, Mariano Trigo^{2

5}, Tony F Heinz^{5

9}, Ju Li^{6

10}, Keith A Nelson¹¹, Edoardo Baldini⁸, Jian Zhou¹², Shambhu Ghimire⁵, David A Reis^{2

5}, Aaron M Lindenberg^{1

2

5}

Affiliations

¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, 94305, USA.
² Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
³ Department of Chemistry, University of Washington, Seattle, WA, 98195, USA.
⁴ Department of Applied Physics, Stanford University, Stanford, CA, 94305, USA.
⁵ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁶ Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
⁷ Laser Science and Technology, SLAC Linear Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁸ Department of Physics, Center for Complex Quantum Systems, The University of Texas at Austin, Austin, TX, 78712, USA.
⁹ E. L. Ginzton Laboratory, Stanford, CA, 94305, USA.
¹⁰ Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
¹¹ Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
¹² Center for Alloy Innovation and Design, State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, 710049, China.

PMID: 40855657
DOI: 10.1002/adma.202510524

Nonresonant Raman Control of Ferroelectric Polarization

Jiaojian Shi et al. Adv Mater. 2025 Nov.

. 2025 Nov;37(44):e10524.

doi: 10.1002/adma.202510524. Epub 2025 Aug 25.

Authors

Affiliations

¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, 94305, USA.
² Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
³ Department of Chemistry, University of Washington, Seattle, WA, 98195, USA.
⁴ Department of Applied Physics, Stanford University, Stanford, CA, 94305, USA.
⁵ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁶ Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
⁷ Laser Science and Technology, SLAC Linear Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁸ Department of Physics, Center for Complex Quantum Systems, The University of Texas at Austin, Austin, TX, 78712, USA.
⁹ E. L. Ginzton Laboratory, Stanford, CA, 94305, USA.
¹⁰ Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
¹¹ Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
¹² Center for Alloy Innovation and Design, State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, 710049, China.

PMID: 40855657
DOI: 10.1002/adma.202510524

Abstract

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.

Keywords: ferroelectricity; impulsive stimulated raman scattering; phase transition.

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References

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Nonresonant Raman Control of Ferroelectric Polarization

Affiliations

Nonresonant Raman Control of Ferroelectric Polarization

Authors

Affiliations

Abstract

References

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