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Title: Optical creation of a supercrystal with three-dimensional nanoscale periodicity

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. Furthermore our results demonstrate opportunities for light-activated pathways to thermally inaccessible and emergent metastable states.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [1];  [1]; ORCiD logo [3];  [1];  [4]; ORCiD logo [4]; ORCiD logo [4];  [4];  [1];  [3];  [3];  [3]; ORCiD logo [5];  [5];  [1]; ORCiD logo [3]; ORCiD logo [1] more »; ORCiD logo [3] « less
  1. Pennsylvania State Univ., University Park, PA (United States)
  2. Center for Nanophase Materials Sciences, Oak Ridge, TN (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. of California, Berkeley, CA (United States)
  5. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1510311
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 18; Journal Issue: 4; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

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, L. -Q., Wen, H., Gopalan, V., and Freeland, J. W. Optical creation of a supercrystal with three-dimensional nanoscale periodicity. United States: N. p., 2019. Web. doi: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, L. -Q., Wen, H., Gopalan, V., & Freeland, J. W. Optical creation of a supercrystal with three-dimensional nanoscale periodicity. United States. doi: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, L. -Q., Wen, H., Gopalan, V., and Freeland, J. W. Mon . "Optical creation of a supercrystal with three-dimensional nanoscale periodicity". United States. doi:10.1038/s41563-019-0311-x.
@article{osti_1510311,
title = {Optical creation of a supercrystal with three-dimensional nanoscale periodicity},
author = {Stoica, V. A. and Laanait, N. and Dai, C. and Hong, Z. and Yuan, Y. and Zhang, Z. and Lei, S. and McCarter, M. R. and Yadav, A. and Damodaran, A. R. and Das, S. and Stone, G. A. and Karapetrova, J. and Walko, D. A. and Zhang, X. and Martin, L. W. and Ramesh, R. and Chen, L. -Q. and Wen, H. and Gopalan, V. and Freeland, J. W.},
abstractNote = {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. Furthermore our results demonstrate opportunities for light-activated pathways to thermally inaccessible and emergent metastable states.},
doi = {10.1038/s41563-019-0311-x},
journal = {Nature Materials},
number = 4,
volume = 18,
place = {United States},
year = {2019},
month = {3}
}

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This content will become publicly available on March 18, 2020
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