<p>When cooling towards a ferroelectric phase transition, collective atomic motions (phonons) slow down (soften) until a static atomic displacement pattern forms, giving rise to spontaneous polarization throughout the material<sup><CitationRef CitationID="CR1">1</CitationRef></sup>. However, in quantum paraelectrics such as strontium titanate (SrTiO<sub>3</sub>), long-range ferroelectric order does not develop at low temperatures due to persistent quantum fluctuations of ionic positions<sup><CitationRef CitationID="CR2">2</CitationRef>,<CitationRef CitationID="CR3">3</CitationRef></sup>. In SrTiO<sub>3</sub>, quantum paraelectricity emerges below <i>T</i><sub>q</sub> ≈ 40 K refs. <sup><CitationRef AdditionalCitationIDS="CR5" CitationID="CR4">4</CitationRef>–<CitationRef CitationID="CR6">6</CitationRef></sup> and is preceded by anomalous phonon dynamics: a transverse acoustic phonon mode partially softens at a finite wavevector, hinting at a modulated state at the nanoscale<sup><CitationRef AdditionalCitationIDS="CR8 CR9 CR10 CR11" CitationID="CR7">7</CitationRef>–<CitationRef CitationID="CR12">12</CitationRef></sup>. The precise real-space structure of SrTiO<sub>3</sub> at low temperature, however, has remained unresolved despite decades of study. Here we directly image the low-temperature polar structure of a SrTiO<sub>3</sub> lamella using cryogenic scanning transmission electron microscopy down to 20 K. High-resolution imaging reveals a spatially fluctuating landscape of nanoscale domains. Below about 105 K, short-range polar domains initially self-organize into a periodic structure extending over tens of nanometres; however, upon entering the quantum paraelectric regime below <i>T</i><sub>q</sub>, the process reverses and the periodically ordered polar nanodomains fragment into smaller clusters. Quantum paraelectricity in SrTiO<sub>3</sub> underlies remarkable properties, including large dielectric permittivity<sup><CitationRef CitationID="CR13">13</CitationRef>,<CitationRef CitationID="CR14">14</CitationRef></sup>, proximity to ferroelectricity<sup><CitationRef CitationID="CR15">15</CitationRef>,<CitationRef CitationID="CR16">16</CitationRef></sup>, multiferroicity<sup><CitationRef CitationID="CR17">17</CitationRef></sup> and unconventional superconductivity<sup><CitationRef AdditionalCitationIDS="CR19" CitationID="CR18">18</CitationRef>–<CitationRef CitationID="CR20">20</CitationRef></sup>. Our visualizations suggest that these phenomena may be linked to complex ordering and disordering of polar nanodomains at low temperature.</p>

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Imaging of nanoscale polar textures in quantum paraelectric SrTiO3

  • Yang Zhang,
  • Suk Hyun Sung,
  • Nishkarsh Agarwal,
  • Maya Gates,
  • Cong Li,
  • Pu Yu,
  • Robert Hovden,
  • Ismail El Baggari

摘要

When cooling towards a ferroelectric phase transition, collective atomic motions (phonons) slow down (soften) until a static atomic displacement pattern forms, giving rise to spontaneous polarization throughout the material1. However, in quantum paraelectrics such as strontium titanate (SrTiO3), long-range ferroelectric order does not develop at low temperatures due to persistent quantum fluctuations of ionic positions2,3. In SrTiO3, quantum paraelectricity emerges below Tq ≈ 40 K refs. 46 and is preceded by anomalous phonon dynamics: a transverse acoustic phonon mode partially softens at a finite wavevector, hinting at a modulated state at the nanoscale712. The precise real-space structure of SrTiO3 at low temperature, however, has remained unresolved despite decades of study. Here we directly image the low-temperature polar structure of a SrTiO3 lamella using cryogenic scanning transmission electron microscopy down to 20 K. High-resolution imaging reveals a spatially fluctuating landscape of nanoscale domains. Below about 105 K, short-range polar domains initially self-organize into a periodic structure extending over tens of nanometres; however, upon entering the quantum paraelectric regime below Tq, the process reverses and the periodically ordered polar nanodomains fragment into smaller clusters. Quantum paraelectricity in SrTiO3 underlies remarkable properties, including large dielectric permittivity13,14, proximity to ferroelectricity15,16, multiferroicity17 and unconventional superconductivity1820. Our visualizations suggest that these phenomena may be linked to complex ordering and disordering of polar nanodomains at low temperature.