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Open Access Publications from the University of California

Optical creation of a supercrystal with three-dimensional nanoscale periodicity.

  • Author(s): Stoica, VA
  • Laanait, N
  • Dai, C
  • Hong, Z
  • Yuan, Y
  • Zhang, Z
  • Lei, S
  • McCarter, MR
  • Yadav, A
  • Damodaran, AR
  • Das, S
  • Stone, GA
  • Karapetrova, J
  • Walko, DA
  • Zhang, X
  • Martin, LW
  • Ramesh, R
  • Chen, L-Q
  • Wen, H
  • Gopalan, V
  • Freeland, JW
  • et al.

Stimulation with ultrafast light pulses can realize and manipulate states of matter with emergent structural, electronic and magnetic phenomena. However, these non-equilibrium phases are often transient and the challenge is to stabilize them as persistent states. Here, we show that atomic-scale PbTiO3/SrTiO3 superlattices, counterpoising strain and polarization states in alternate layers, are converted by sub-picosecond optical pulses to a supercrystal phase. This phase persists indefinitely under ambient conditions, has not been created via equilibrium routes, and can be erased by heating. X-ray scattering and microscopy show this unusual phase consists of a coherent three-dimensional structure with polar, strain and charge-ordering periodicities of up to 30 nm. By adjusting only dielectric properties, the phase-field model describes this emergent phase as a photo-induced charge-stabilized supercrystal formed from a two-phase equilibrium state. Our results demonstrate opportunities for light-activated pathways to thermally inaccessible and emergent metastable states.

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