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Title: High Tc layered ferrielectric crystals by coherent spinodal decomposition

Research in the rapidly-developing field of 2D-electronic materials has thus far been focused on metallic and semiconducting materials. However, complementary dielectric materials such as non-linear dielectrics are needed to enable realistic device architectures. Candidate materials require tunable dielectric properties and pathways for heterostructure assembly. Here we report on a family of cation-deficient transition metal thiophosphates whose unique chemistry makes them a viable prospect for these applications. In these materials, naturally occurring ferrielectric heterostructures composed of centrosymmetric In4/3P2S6 and ferrielectrically-active CuInP2S6 are realized by controllable chemical phase separation in van-der-Waals bonded single crystals. CuInP2S6 by itself is a layered ferrielectric with Tc just over room-temperature which rapidly decreases with homogenous doping. Surprisingly, in our composite materials, the ferrielectric Tc of the polar CuInP2S6 phase increases. This effect is enabled by unique spinodal decomposition that retains the overall van-der-Waals layered morphology of the crystal, but chemically separates CuInP2S6 and In4/3P2S6 within each layer. The average spatial periodicity of the distinct chemical phases can be finely controlled by altering the composition and/or synthesis conditions. One intriguing prospect for such layered spinodal alloys is large volume synthesis of 2D in-plane heterostructures with periodically alternating polar and non-polar phases.
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [1] ;  [1] ;  [1] ;  [3]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
  3. ORNL
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 1936-0851
American Chemical Society
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). High Temperature Materials Lab. (HTML); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Joint Institute for Computational Sciences (JICS)
Sponsoring Org:
Country of Publication:
United States
OSTI Identifier: