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<p>A fundamental understanding of the interplay between lattice structure, polarization and electrons is pivotal to the optical control of ferroelectrics. The interaction between light and matter enables the remote and wireless control of the ferroelectric polarization on the picosecond timescale, while inducing strain, i.e., lattice deformation. At equilibrium, the ferroelectric polarization is proportional to the strain, and is typically assumed to be so also out of equilibrium. Decoupling the polarization from the strain would remove the constraint of sample design and provide an effective knob to manipulate the polarization by light. Here, upon above-bandgap laser excitation of the prototypical ferroelectric BaTiO<sub>3</sub>, we induce and measure an ultrafast decoupling between polarization and strain that begins within 350 fs, by softening Ti-O bonds via charge transfer, and lasts for several tens of picoseconds. We show that the ferroelectric polarization out of equilibrium is mainly determined by photoexcited electrons, instead of the strain.</p>

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Ultrafast decoupling of polarization and strain in ferroelectric BaTiO3

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月26日

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  • Le Phuong Hoang,
  • David Pesquera,
  • Gerard N. Hinsley,
  • Robert Carley,
  • Laurent Mercadier,
  • Martin Teichmann,
  • Elena Martina Unterleutner,
  • Daniel Knez,
  • Martina Dienstleder,
  • Saptam Ganguly,
  • Teguh Citra Asmara,
  • Giacomo Merzoni,
  • Sergii Parchenko,
  • Justine Schlappa,
  • Zhong Yin,
  • José Manuel Caicedo Roque,
  • José Santiso,
  • Irena Spasojevic,
  • Cammille Carinan,
  • Tien-Lin Lee,
  • Kai Rossnagel,
  • Jörg Zegenhagen,
  • Gustau Catalan,
  • Ivan A. Vartanyants,
  • Andreas Scherz,
  • Giuseppe Mercurio

摘要

A fundamental understanding of the interplay between lattice structure, polarization and electrons is pivotal to the optical control of ferroelectrics. The interaction between light and matter enables the remote and wireless control of the ferroelectric polarization on the picosecond timescale, while inducing strain, i.e., lattice deformation. At equilibrium, the ferroelectric polarization is proportional to the strain, and is typically assumed to be so also out of equilibrium. Decoupling the polarization from the strain would remove the constraint of sample design and provide an effective knob to manipulate the polarization by light. Here, upon above-bandgap laser excitation of the prototypical ferroelectric BaTiO3, we induce and measure an ultrafast decoupling between polarization and strain that begins within 350 fs, by softening Ti-O bonds via charge transfer, and lasts for several tens of picoseconds. We show that the ferroelectric polarization out of equilibrium is mainly determined by photoexcited electrons, instead of the strain.