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Optical creation of a supercrystal with three-dimensional nanoscale periodicity

Journal Article · · Nature Materials
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  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)
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.
Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; AC05-00OR22725
OSTI ID:
1510311
Alternate ID(s):
OSTI ID: 1542390
OSTI ID: 1862165
Journal Information:
Nature Materials, Journal Name: Nature Materials Journal Issue: 4 Vol. 18; ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Role of temperature-dependent electron trapping dynamics in the optically driven nanodomain transformation in a PbTiO 3 /SrTiO 3 superlattice journal January 2020
Dynamics of a Persistent Insulator-to-Metal Transition in Strained Manganite Films journal December 2019
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Design and Manipulation of Ferroic Domains in Complex Oxide Heterostructures journal September 2019
Design and Manipulation of Ferroic Domains in Complex Oxide Heterostructures text January 2019
Role of temperature-dependent electron trapping dynamics in the optically driven nanodomain transformation in a PbTiO${_3}$/SrTiO${_3}$ superlattice text January 2019