Revealing Fast Cu-Ion Transport and Enhanced Conductivity at the CuInP2S6-In4/3P2S6Heterointerface

Marti Checa; Xin Jin; Ruben Millan-Solsona; Sabine M. Neumayer; Michael A. Susner; Michael A. McGuire; Andrew O'Hara; Gabriel Gomila; Petro Maksymovych; Sokrates T. Pantelides; Liam Collins

doi:10.1021/acsnano.2c06992

Revealing Fast Cu-Ion Transport and Enhanced Conductivity at the CuInP₂S₆-In_4/3P₂S₆Heterointerface

Marti Checa, Xin Jin, Ruben Millan-Solsona, Sabine M. Neumayer, Michael A. Susner, Michael A. McGuire, Andrew O'Hara, Gabriel Gomila, Petro Maksymovych, Sokrates T. Pantelides, Liam Collins

Research output: Contribution to journal › Article › peer-review

14 Scopus citations

Abstract

Van der Waals layered ferroelectrics, such as CuInP2S6 (CIPS), offer a versatile platform for miniaturization of ferroelectric device technologies. Control of the targeted composition and kinetics of CIPS synthesis enables the formation of stable self-assembled heterostructures of ferroelectric CIPS and nonferroelectric In4/3P2S6 (IPS). Here, we use quantitative scanning probe microscopy methods combined with density functional theory (DFT) to explore in detail the nanoscale variability in dynamic functional properties of the CIPS-IPS heterostructure. We report evidence of fast ionic transport which mediates an appreciable out-of-plane electromechanical response of the CIPS surface in the paraelectric phase. Further, we map the nanoscale dielectric and ionic conductivity properties as we thermally stimulate the ferroelectric-paraelectric phase transition, recovering the local dielectric behavior during this phase transition. Finally, aided by DFT, we reveal a substantial and tunable conductivity enhancement at the CIPS/IPS interface, indicating the possibility of engineering its interfacial properties for next generation device applications.

Original language	English
Pages (from-to)	15347-15357
Number of pages	11
Journal	ACS Nano
Volume	16
Issue number	9
DOIs	https://doi.org/10.1021/acsnano.2c06992
State	Published - Sep 27 2022

Funding

Experimental research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Theoretical work at Vanderbilt University (X.J., A.O., S.T.P.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division grant no. DE-FG02-09ER46554 and by the McMinn Endowment at Vanderbilt University. This manuscript has been authored by UT-Battelle, LLC, under contract no. DEAC0500OR22725 with the U.S. Department of Energy. Additional support for sample synthesis and manuscript preparation was supplied by the United States Air Force Office of Scientific Research (AFOSR) LRIR 18RQCOR100 and AOARD-MOST Grant Number F4GGA21207H002. G.G. and R.M.-S. acknowledge support from the Spanish Ministerio de Economıa, Industria y Competitividad and EU FEDER through grant no. PID2019-110210GB-I00.

Keywords

copper indium thiophosphate
ferroelectrics
ionic conductor
phase transition
piezoresponse force microscopy
scanning dielectric microscopy

Access to Document

10.1021/acsnano.2c06992

Cite this

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title = "Revealing Fast Cu-Ion Transport and Enhanced Conductivity at the CuInP2S6-In4/3P2S6Heterointerface",

abstract = "Van der Waals layered ferroelectrics, such as CuInP2S6 (CIPS), offer a versatile platform for miniaturization of ferroelectric device technologies. Control of the targeted composition and kinetics of CIPS synthesis enables the formation of stable self-assembled heterostructures of ferroelectric CIPS and nonferroelectric In4/3P2S6 (IPS). Here, we use quantitative scanning probe microscopy methods combined with density functional theory (DFT) to explore in detail the nanoscale variability in dynamic functional properties of the CIPS-IPS heterostructure. We report evidence of fast ionic transport which mediates an appreciable out-of-plane electromechanical response of the CIPS surface in the paraelectric phase. Further, we map the nanoscale dielectric and ionic conductivity properties as we thermally stimulate the ferroelectric-paraelectric phase transition, recovering the local dielectric behavior during this phase transition. Finally, aided by DFT, we reveal a substantial and tunable conductivity enhancement at the CIPS/IPS interface, indicating the possibility of engineering its interfacial properties for next generation device applications.",

keywords = "copper indium thiophosphate, ferroelectrics, ionic conductor, phase transition, piezoresponse force microscopy, scanning dielectric microscopy",

author = "Marti Checa and Xin Jin and Ruben Millan-Solsona and Neumayer, {Sabine M.} and Susner, {Michael A.} and McGuire, {Michael A.} and Andrew O'Hara and Gabriel Gomila and Petro Maksymovych and Pantelides, {Sokrates T.} and Liam Collins",

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AU - Neumayer, Sabine M.

AU - Susner, Michael A.

AU - McGuire, Michael A.

AU - O'Hara, Andrew

AU - Gomila, Gabriel

AU - Maksymovych, Petro

AU - Pantelides, Sokrates T.

AU - Collins, Liam

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AB - Van der Waals layered ferroelectrics, such as CuInP2S6 (CIPS), offer a versatile platform for miniaturization of ferroelectric device technologies. Control of the targeted composition and kinetics of CIPS synthesis enables the formation of stable self-assembled heterostructures of ferroelectric CIPS and nonferroelectric In4/3P2S6 (IPS). Here, we use quantitative scanning probe microscopy methods combined with density functional theory (DFT) to explore in detail the nanoscale variability in dynamic functional properties of the CIPS-IPS heterostructure. We report evidence of fast ionic transport which mediates an appreciable out-of-plane electromechanical response of the CIPS surface in the paraelectric phase. Further, we map the nanoscale dielectric and ionic conductivity properties as we thermally stimulate the ferroelectric-paraelectric phase transition, recovering the local dielectric behavior during this phase transition. Finally, aided by DFT, we reveal a substantial and tunable conductivity enhancement at the CIPS/IPS interface, indicating the possibility of engineering its interfacial properties for next generation device applications.

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