4.8 Article

Light-Driven Ultrafast Polarization Manipulation in a Relaxor Ferroelectric

Journal

NANO LETTERS
Volume 22, Issue 23, Pages 9275-9282

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c02706

Keywords

ferroelectrics; structural dynamics; ultrafast; electron diffraction

Funding

  1. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC-0012375]
  2. DOE BES SUF Division Accelerator & Detector RD program
  3. LCLS Facility
  4. SLAC [DE-AC02-05-CH11231, DE-AC02- 76SF00515]
  5. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
  6. Army Research Office [W911NF-21-1-0118]
  7. National Science Foundation [DMR-2102895]
  8. Collaborative for Hierarchical Agile and Responsive Materials (CHARM) [W911NF-19-2-0119]
  9. National Science Foundation (NSF) [DMR-1744213]
  10. Computational Materials Sciences Program - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0020145]

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This study presents the first investigation on the ultrafast dynamics and reconfigurability of polarization in freestanding films of a typical relaxor ferroelectric using femtosecond-resolution electron-scattering techniques. The results demonstrate that femtosecond light pulses can induce changes in both the magnitude and direction of the polarization vector within polar nanodomains on a picosecond time scale. These findings offer new possibilities for dynamically reconfigurable control of polarization in nanoscale relaxor ferroelectrics.
Relaxor ferroelectrics have been intensely studied for decades based on their unique electromechanical responses which arise from local structural heterogeneity involving polar nanoregions or domains. Here, we report first studies of the ultrafast dynamics and reconfigurability of the polarization in freestanding films of the prototypical relaxor 0.68PbMg1/3Nb2/3O3- 0.32PbTiO3 (PMN-0.32PT) by probing its atomic-scale response via femtosecond-resolution, electron-scattering approaches. By combining these structural measurements with dynamic phase-field simulations, we show that femtosecond light pulses drive a change in both the magnitude and direction of the polarization vector within polar nanodomains on few-picosecond time scales. This study defines new opportunities for dynamic reconfigurable control of the polarization in nanoscale relaxor ferroelectrics.

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