Nonresonant Raman Control of Ferroelectric Polarization

Jiaojian Shi; Christian Heide; Haowei Xu; Yuejun Shen; Meredith Henstridge; Isabel Sedwick; Anudeep Mangu; Xinyue Peng; Shangjie Zhang; Mariano Trigo; Tony F. Heinz; Ju Li; Keith A. Nelson; Edoardo Baldini; Jian Zhou; Shambhu Ghimire; David A. Reis; Aaron M. Lindenberg

doi:10.1002/adma.202510524

Nonresonant Raman Control of Ferroelectric Polarization

Jiaojian Shi^* (Co-first Author), Christian Heide (Co-first Author), Haowei Xu (Co-first Author), Yuejun Shen (Co-first Author), Meredith Henstridge, Isabel Sedwick, Anudeep Mangu, Xinyue Peng, Shangjie Zhang, Mariano Trigo, Tony F. Heinz, Ju Li, Keith A. Nelson, Edoardo Baldini, Jian Zhou, Shambhu Ghimire, David A. Reis, Aaron M. Lindenberg^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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. © 2025 Wiley-VCH GmbH.

Original language	English
Article number	e10524
Number of pages	8
Journal	Advanced Materials
Volume	37
Issue number	44
Online published	25 Aug 2025
DOIs	https://doi.org/10.1002/adma.202510524
Publication status	Published - 6 Nov 2025
Externally published	Yes

Funding

This work was supported by the US Department of Energy (DOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under contract no. DE-AC02-76SF00515. I.S. and J.S. acknowledge the start-up funding provided by the University of Washington. H.X. and J.L. acknowledge support by an Office of Naval Research MURI through grant #N00014-17-1-2661. Work at UT Austin was supported by the National Science Foundation under grant DMR-2308817 (to X.P. for data taking), the Air Force Office of Scientific Research under Young Investigator Program award FA9550-24-1-0097 (to S.Z. for data taking), and the ARL-UT Austin Cooperative Agreement W911NF-21-2-0185 (to E.B. for data interpretation and supervision). J.Z. acknowledges the support by the National Natural Science Foundation of China under grant No. 21903063. C.H. acknowledges support from the U.S. Department of Energy, Office of Science through the AMOS program and the Alexander von Humboldt Research Fellowship. S.G. acknowledges support from the U.S. Department of Energy, Office of Science through the AMOS program. K.A.N. acknowledges support from the U.S. Department of Energy, Office of Basic Energy Sciences, under Award No. DE-SC0019126.

Research Keywords

ferroelectricity
impulsive stimulated raman scattering
phase transition

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title = "Nonresonant Raman Control of Ferroelectric Polarization",

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. {\textcopyright} 2025 Wiley-VCH GmbH.",

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author = "Jiaojian Shi and Christian Heide and Haowei Xu and Yuejun Shen and Meredith Henstridge and Isabel Sedwick and Anudeep Mangu and Xinyue Peng and Shangjie Zhang and Mariano Trigo and Heinz, {Tony F.} and Ju Li and Nelson, {Keith A.} and Edoardo Baldini and Jian Zhou and Shambhu Ghimire and Reis, {David A.} and Lindenberg, {Aaron M.}",

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doi = "10.1002/adma.202510524",

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T1 - Nonresonant Raman Control of Ferroelectric Polarization

AU - Shi, Jiaojian

AU - Heide, Christian

AU - Xu, Haowei

AU - Shen, Yuejun

AU - Henstridge, Meredith

AU - Sedwick, Isabel

AU - Mangu, Anudeep

AU - Peng, Xinyue

AU - Zhang, Shangjie

AU - Trigo, Mariano

AU - Heinz, Tony F.

AU - Li, Ju

AU - Nelson, Keith A.

AU - Baldini, Edoardo

AU - Zhou, Jian

AU - Ghimire, Shambhu

AU - Reis, David A.

AU - Lindenberg, Aaron M.

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Y1 - 2025/11/6

N2 - 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. © 2025 Wiley-VCH GmbH.

AB - 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. © 2025 Wiley-VCH GmbH.

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KW - impulsive stimulated raman scattering

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Nonresonant Raman Control of Ferroelectric Polarization

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