Optical creation of a supercrystal with three-dimensional nanoscale periodicity

V. A. Stoica, N. Laanait, C. Dai, Z. Hong, Y. Yuan, Z. Zhang, S. Lei, M. R. McCarter, A. Yadav, A. R. Damodaran, S. Das, G. A. Stone, J. Karapetrova, D. A. Walko, X. Zhang, L. W. Martin, R. Ramesh, Long-qing Chen, H. Wen, Venkatraman GopalanJ. W. Freeland

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

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 PbTiO 3 /SrTiO 3 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.

Original languageEnglish (US)
Pages (from-to)377-383
Number of pages7
JournalNature Materials
Volume18
Issue number4
DOIs
StatePublished - Apr 1 2019

Fingerprint

periodic variations
Superlattices
pulses
X ray scattering
stimulation
Phase equilibria
metastable state
Dielectric properties
superlattices
dielectric properties
Laser pulses
Microscopic examination
adjusting
routes
Polarization
microscopy
Heating
heating
polarization
scattering

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering

Cite this

Stoica, V. A., Laanait, N., Dai, C., Hong, Z., Yuan, Y., Zhang, Z., ... Freeland, J. W. (2019). Optical creation of a supercrystal with three-dimensional nanoscale periodicity. Nature Materials, 18(4), 377-383. https://doi.org/10.1038/s41563-019-0311-x
Stoica, V. A. ; Laanait, N. ; Dai, C. ; Hong, Z. ; Yuan, Y. ; Zhang, Z. ; Lei, S. ; McCarter, M. R. ; Yadav, A. ; Damodaran, A. R. ; Das, S. ; Stone, G. A. ; Karapetrova, J. ; Walko, D. A. ; Zhang, X. ; Martin, L. W. ; Ramesh, R. ; Chen, Long-qing ; Wen, H. ; Gopalan, Venkatraman ; Freeland, J. W. / Optical creation of a supercrystal with three-dimensional nanoscale periodicity. In: Nature Materials. 2019 ; Vol. 18, No. 4. pp. 377-383.
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abstract = "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 PbTiO 3 /SrTiO 3 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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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, Wen, H, Gopalan, V & Freeland, JW 2019, 'Optical creation of a supercrystal with three-dimensional nanoscale periodicity', Nature Materials, vol. 18, no. 4, pp. 377-383. https://doi.org/10.1038/s41563-019-0311-x

Optical creation of a supercrystal with three-dimensional nanoscale periodicity. / Stoica, V. A.; Laanait, N.; Dai, C.; Hong, Z.; Yuan, Y.; Zhang, Z.; Lei, S.; McCarter, M. R.; Yadav, A.; Damodaran, A. R.; Das, S.; Stone, G. A.; Karapetrova, J.; Walko, D. A.; Zhang, X.; Martin, L. W.; Ramesh, R.; Chen, Long-qing; Wen, H.; Gopalan, Venkatraman; Freeland, J. W.

In: Nature Materials, Vol. 18, No. 4, 01.04.2019, p. 377-383.

Research output: Contribution to journalArticle

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T1 - Optical creation of a supercrystal with three-dimensional nanoscale periodicity

AU - Stoica, V. A.

AU - Laanait, N.

AU - Dai, C.

AU - Hong, Z.

AU - Yuan, Y.

AU - Zhang, Z.

AU - Lei, S.

AU - McCarter, M. R.

AU - Yadav, A.

AU - Damodaran, A. R.

AU - Das, S.

AU - Stone, G. A.

AU - Karapetrova, J.

AU - Walko, D. A.

AU - Zhang, X.

AU - Martin, L. W.

AU - Ramesh, R.

AU - Chen, Long-qing

AU - Wen, H.

AU - Gopalan, Venkatraman

AU - Freeland, J. W.

PY - 2019/4/1

Y1 - 2019/4/1

N2 - 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 PbTiO 3 /SrTiO 3 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.

AB - 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 PbTiO 3 /SrTiO 3 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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