Nonresonant Raman control of ferroelectric polarization

Fuente: arXiv
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Main Authors: Shi, Jiaojian, Heide, Christian, Xu, Haowei, Shen, Yuejun, Henstridge, Meredith, Sedwick, Isabel, Mangu, Anudeep, Peng, Xinyue, Zhang, Shangjie, Trigo, Mariano, Heinz, Tony F., Li, Ju, Nelson, Keith A., Baldini, Edoardo, Zhou, Jian, Ghimire, Shambhu, Reis, David A., Lindenberg, Aaron M.
Format: Preprint
Published: 2024
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author Shi, Jiaojian
Heide, Christian
Xu, Haowei
Shen, Yuejun
Henstridge, Meredith
Sedwick, Isabel
Mangu, Anudeep
Peng, Xinyue
Zhang, Shangjie
Trigo, Mariano
Heinz, Tony F.
Li, Ju
Nelson, Keith A.
Baldini, Edoardo
Zhou, Jian
Ghimire, Shambhu
Reis, David A.
Lindenberg, Aaron M.
author_facet Shi, Jiaojian
Heide, Christian
Xu, Haowei
Shen, Yuejun
Henstridge, Meredith
Sedwick, Isabel
Mangu, Anudeep
Peng, Xinyue
Zhang, Shangjie
Trigo, Mariano
Heinz, Tony F.
Li, Ju
Nelson, Keith A.
Baldini, Edoardo
Zhou, Jian
Ghimire, Shambhu
Reis, David A.
Lindenberg, Aaron M.
contents Important advances have recently been 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 has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been 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.
format Preprint
id arxiv_https___arxiv_org_abs_2411_10131
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Nonresonant Raman control of ferroelectric polarization
Shi, Jiaojian
Heide, Christian
Xu, Haowei
Shen, Yuejun
Henstridge, Meredith
Sedwick, Isabel
Mangu, Anudeep
Peng, Xinyue
Zhang, Shangjie
Trigo, Mariano
Heinz, Tony F.
Li, Ju
Nelson, Keith A.
Baldini, Edoardo
Zhou, Jian
Ghimire, Shambhu
Reis, David A.
Lindenberg, Aaron M.
Optics
Materials Science
Important advances have recently been 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 has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been 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.
title Nonresonant Raman control of ferroelectric polarization
topic Optics
Materials Science
url https://arxiv.org/abs/2411.10131