Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes

Liu, Fucai; You, Lu; Seyler, Kyle L.; Li, Xiaobao; Yu, Peng; Lin, Junhao; Wang, Xuewen; Zhou, Jiadong; Wang, Hong; He, Haiyong; Pantelides, Sokrates T.; Zhou, Wu; Sharma, Pradeep; Xu, Xiaodong; Ajayan, Pulickel M.; Wang, Junling; Liu, Zheng

doi:10.1038/ncomms12357

Title: Room-temperature ferroelectricity in CuInP₂S₆ ultrathin flakes

Abstract

In this study, two-dimensional (2D) materials have emerged as promising candidates for various optoelectronic applications based on their diverse electronic properties, ranging from insulating to superconducting. However, cooperative phenomena such as ferroelectricity in the 2D limit have not been well explored. Here, we report room-temperature ferroelectricity in 2D CuInP₂S₆ (CIPS) with a transition temperature of ~320 K. Switchable polarization is observed in thin CIPS of ~4 nm. To demonstrate the potential of this 2D ferroelectric material, we prepare a van der Waals (vdW) ferroelectric diode formed by CIPS/Si heterostructure, which shows good memory behaviour with on/off ratio of ~100. The addition of ferroelectricity to the 2D family opens up possibilities for numerous novel applications, including sensors, actuators, non-volatile memory devices, and various vdW heterostructures based on 2D ferroelectricity.

Authors:

Liu, Fucai ^[1];

^[1]; Seyler, Kyle L. ^[2]; Li, Xiaobao ^[3]; Yu, Peng ^[1]; Lin, Junhao ^[4]; Wang, Xuewen ^[1]; Zhou, Jiadong ^[1]; Wang, Hong ^[1]; He, Haiyong ^[1];

^[5];

^[6]; Sharma, Pradeep ^[7];

^[2]; Ajayan, Pulickel M. ^[8];

^[1]; Liu, Zheng ^[9]

Nanyang Technological Univ. (Singapore)
Univ. of Washington, Seattle, WA (United States)
Hefei Univ. of Technology, Hefei (China)
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); National Institute of Advanced Industrial Science and Technology, Tsukuba (Japan)
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Houston, Houston, TX (United States)
Rice Univ., Houston, TX (United States)
Nanyang Technological Univ. (Singapore); CINTRA CNRS/NTU/THALES (Singapore)

Publication Date:: Thu Aug 11 00:00:00 EDT 2016

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1331101

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 7; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats


                    Liu, Fucai, You, Lu, Seyler, Kyle L., Li, Xiaobao, Yu, Peng, Lin, Junhao, Wang, Xuewen, Zhou, Jiadong, Wang, Hong, He, Haiyong, Pantelides, Sokrates T., Zhou, Wu, Sharma, Pradeep, Xu, Xiaodong, Ajayan, Pulickel M., Wang, Junling, and Liu, Zheng. Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes.  United States: N. p., 2016. 
Web.  doi:10.1038/ncomms12357.

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                    Liu, Fucai, You, Lu, Seyler, Kyle L., Li, Xiaobao, Yu, Peng, Lin, Junhao, Wang, Xuewen, Zhou, Jiadong, Wang, Hong, He, Haiyong, Pantelides, Sokrates T., Zhou, Wu, Sharma, Pradeep, Xu, Xiaodong, Ajayan, Pulickel M., Wang, Junling, & Liu, Zheng. Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes.  United States.  https://doi.org/10.1038/ncomms12357

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                    Liu, Fucai, You, Lu, Seyler, Kyle L., Li, Xiaobao, Yu, Peng, Lin, Junhao, Wang, Xuewen, Zhou, Jiadong, Wang, Hong, He, Haiyong, Pantelides, Sokrates T., Zhou, Wu, Sharma, Pradeep, Xu, Xiaodong, Ajayan, Pulickel M., Wang, Junling, and Liu, Zheng. Thu .  
"Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes".  United States.  https://doi.org/10.1038/ncomms12357.  https://www.osti.gov/servlets/purl/1331101.

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@article{osti_1331101,

  title        = {Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes},

  author       = {Liu, Fucai and You, Lu and Seyler, Kyle L. and Li, Xiaobao and Yu, Peng and Lin, Junhao and Wang, Xuewen and Zhou, Jiadong and Wang, Hong and He, Haiyong and Pantelides, Sokrates T. and Zhou, Wu and Sharma, Pradeep and Xu, Xiaodong and Ajayan, Pulickel M. and Wang, Junling and Liu, Zheng},

  abstractNote = {In this study, two-dimensional (2D) materials have emerged as promising candidates for various optoelectronic applications based on their diverse electronic properties, ranging from insulating to superconducting. However, cooperative phenomena such as ferroelectricity in the 2D limit have not been well explored. Here, we report room-temperature ferroelectricity in 2D CuInP2S6 (CIPS) with a transition temperature of ~320 K. Switchable polarization is observed in thin CIPS of ~4 nm. To demonstrate the potential of this 2D ferroelectric material, we prepare a van der Waals (vdW) ferroelectric diode formed by CIPS/Si heterostructure, which shows good memory behaviour with on/off ratio of ~100. The addition of ferroelectricity to the 2D family opens up possibilities for numerous novel applications, including sensors, actuators, non-volatile memory devices, and various vdW heterostructures based on 2D ferroelectricity.},

  doi          = {10.1038/ncomms12357},

  journal      = {Nature Communications},

  number       = ,

  volume       = 7,

  place        = {United States},

  year         = {Thu Aug 11 00:00:00 EDT 2016},

  month        = {Thu Aug 11 00:00:00 EDT 2016}

}

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Chen, Liufang; Li, Yongqiang; Li, Chuanfu
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Sun, Zhi-Zheng; Xun, Wei; Jiang, Li
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Chang, Kai; Miller, Brandon J.; Yang, Hao
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Lin, Ling-Fang; Zhang, Yang; Moreo, Adriana
Physical Review Letters, Vol. 123, Issue 6
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Lin, Ling-Fang; Zhang, Yang; Moreo, Adriana
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Zheng, Changxi; Yu, Lei; Zhu, Lin
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You, Lu; Zhang, Yang; Zhou, Shuang
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Ferroelectric or non-ferroelectric: why so many materials exhibit ferroelectricity on the nanoscale
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Vasudevan, Rama K.; Balke, Nina; Maksymovych, Peter
arXiv
DOI: 10.48550/arxiv.1701.01128

Proton-transfer Ferroelectricity / Multiferroicity in Rutile Oxyhydroxides
text, January 2018

Wu, Menghao; Duan, Tianci; Lu, Chengliang
arXiv
DOI: 10.48550/arxiv.1811.00091

Frustrated Dipole Order Induces Noncollinear Proper Ferrielectricity in Two Dimensions
text, January 2019

Lin, Ling-Fang; Zhang, Yang; Moreo, Adriana
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journal, November 2018

Yang, Qing; Zhong, Tingting; Tu, Zhengyuan
Advanced Science, Vol. 6, Issue 1
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Quinuclidinium salt ferroelectric thin-film with duodecuple-rotational polarization-directions
journal, April 2017

You, Yu-Meng; Tang, Yuan-Yuan; Li, Peng-Fei
Nature Communications, Vol. 8, Issue 1
DOI: 10.1038/ncomms14934

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Zheng, Changxi; Yu, Lei; Zhu, Lin
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You, Lu; Zhang, Yang; Zhou, Shuang
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DOI: 10.1126/sciadv.aav3780

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Title: Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes

Abstract

Citation Formats

Ferroelectricity at the Nanoscale: Local Polarization in Oxide Thin Films and Heterostructures journal, January 2004

Ferroelectric tunnel junctions for information storage and processing journal, July 2014

Physics of thin-film ferroelectric oxides journal, October 2005

Strain Tuning of Ferroelectric Thin Films journal, August 2007

Extrinsic and Intrinsic Charge Trapping at the Graphene/Ferroelectric Interface journal, August 2014

Interface Physics in Complex Oxide Heterostructures journal, March 2011

Strongly enhanced charge-density-wave order in monolayer NbSe2 journal, July 2015

Bandgap opening in few-layered monoclinic MoTe2 journal, May 2015

Black phosphorus field-effect transistors journal, March 2014

CuInP 2 S 6 Room Temperature Layered Ferroelectric journal, May 2015

Paraelectric-Ferroelectric Transition in the Lamellar Thiophosphate CuInP2S6 journal, September 1994

Room-temperature crystal structure of the layered phase CuIInIIIP2S6 journal, March 1995

Ferrielectric ordering in lamellar CuInP 2 S 6 journal, November 1997

Piezoresponse force microscopy and recent advances in nanoscale studies of ferroelectrics journal, January 2006

Scaling of structure and electrical properties in ultrathin epitaxial ferroelectric heterostructures journal, September 2006

The piezoresponse force microscopy of surface layers and thin films: Effective response and resolution function journal, October 2007

Flexoelectric rotation of polarization in ferroelectric thin films journal, October 2011

Critical thickness for ferroelectricity in perovskite ultrathin films journal, April 2003

Ultrathin limit and dead-layer effects in local polarization switching of BiFeO 3 journal, January 2012

Interface-induced nonswitchable domains in ferroelectric thin films journal, August 2014

Origin of the dielectric dead layer in nanoscale capacitors journal, October 2006

The Role of Electrochemical Phenomena in Scanning Probe Microscopy of Ferroelectric Thin Films journal, June 2011

Switchable Induced Polarization in LaAlO 3 /SrTiO 3 Heterostructures journal, January 2012

Probing Surface and Bulk Electrochemical Processes on the LaAlO 3 –SrTiO 3 Interface journal, April 2012

Probing Ferroelectrics Using Optical Second Harmonic Generation journal, August 2011

Second harmonic generation in the lamellar ferrielectric CuInP2S6 journal, August 2000

Solid-state memories based on ferroelectric tunnel junctions journal, December 2011

Theory of polarization of crystalline solids journal, January 1993

Ferroelectricity at the Nanoscale: Local Polarization in Oxide Thin Films and Heterostructures journal, April 2004

Strongly enhanced charge-density-wave order in monolayer NbSe$_2$ text, January 2015

Physics of thin-film ferroelectric oxides text, January 2005

Room-temperature crystal structure of the layered phase CuIInIIIP2S6 journal, March 1995

Switchable Induced Polarization in LaAlO 3 /SrTiO 3 Heterostructures journal, January 2012

The Role of Electrochemical Phenomena in Scanning Probe Microscopy of Ferroelectric Thin Films journal, June 2011

Ferroelectric tunnel junctions for information storage and processing journal, July 2014

Interface-induced nonswitchable domains in ferroelectric thin films journal, August 2014

Flexoelectric rotation of polarization in ferroelectric thin films journal, October 2011

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal, September 2009

Probing Ferroelectrics Using Optical Second Harmonic Generation journal, August 2011

Ferroelectricity at the Nanoscale: Local Polarization in Oxide Thin Films and Heterostructures journal, January 2004

The Piezoresponse Force Microscopy of surface layers and thin films: effective response and resolution function text, January 2007

Physics of thin-film ferroelectric oxides text, January 2005

Room‐Temperature Ferroelectricity in Hexagonally Layered α‐In 2 Se 3 Nanoflakes down to the Monolayer Limit journal, October 2018

Metal Thio- and Selenophosphates as Multifunctional van der Waals Layered Materials journal, August 2017

In-Plane Ferroelectricity in Thin Flakes of Van der Waals Hybrid Perovskite journal, October 2018

Gate‐Tunable and Multidirection‐Switchable Memristive Phenomena in a Van Der Waals Ferroelectric journal, May 2019

Spintronics of Hybrid Organic–Inorganic Perovskites: Miraculous Basis of Integrated Optoelectronic Devices journal, June 2019

Design of Single-Molecule Multiferroics for Efficient Ultrahigh-Density Nonvolatile Memories journal, November 2018

Recent Progress in Two‐Dimensional Ferroelectric Materials journal, November 2019

Intrinsic Dipole Coupling in 2D van der Waals Ferroelectrics for Gate‐Controlled Switchable Rectifier journal, November 2019

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Metal Phosphorous Trichalcogenides (MPCh 3 ): From Synthesis to Contemporary Energy Challenges journal, July 2019

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Nanocrystalline Cellulose for Anisotropic Magnetoelectric Composites journal, May 2018

Thickness‐Dependent In‐Plane Polarization and Structural Phase Transition in van der Waals Ferroelectric CuInP 2 S 6 journal, December 2019

The rise of two-dimensional van der Waals ferroelectrics journal, May 2018

Progress and prospects in low-dimensional multiferroic materials journal, January 2019

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Title: Room-temperature ferroelectricity in CuInP₂S₆ ultrathin flakes

Ferroelectricity at the Nanoscale: Local Polarization in Oxide Thin Films and Heterostructures
journal, January 2004

Ferroelectric tunnel junctions for information storage and processing
journal, July 2014

Physics of thin-film ferroelectric oxides
journal, October 2005

Strain Tuning of Ferroelectric Thin Films
journal, August 2007

Extrinsic and Intrinsic Charge Trapping at the Graphene/Ferroelectric Interface
journal, August 2014

Interface Physics in Complex Oxide Heterostructures
journal, March 2011

Strongly enhanced charge-density-wave order in monolayer NbSe₂
journal, July 2015

Bandgap opening in few-layered monoclinic MoTe2
journal, May 2015

Black phosphorus field-effect transistors
journal, March 2014

CuInP ₂ S ₆ Room Temperature Layered Ferroelectric
journal, May 2015

Paraelectric-Ferroelectric Transition in the Lamellar Thiophosphate CuInP2S6
journal, September 1994

Room-temperature crystal structure of the layered phase CuIInIIIP2S6
journal, March 1995

Ferrielectric ordering in lamellar ${CuInP}_{2} S_{6}$
journal, November 1997

Piezoresponse force microscopy and recent advances in nanoscale studies of ferroelectrics
journal, January 2006

Scaling of structure and electrical properties in ultrathin epitaxial ferroelectric heterostructures
journal, September 2006

The piezoresponse force microscopy of surface layers and thin films: Effective response and resolution function
journal, October 2007

Flexoelectric rotation of polarization in ferroelectric thin films
journal, October 2011

Critical thickness for ferroelectricity in perovskite ultrathin films
journal, April 2003

Ultrathin limit and dead-layer effects in local polarization switching of BiFeO $_{3}$
journal, January 2012

Interface-induced nonswitchable domains in ferroelectric thin films
journal, August 2014

Origin of the dielectric dead layer in nanoscale capacitors
journal, October 2006

The Role of Electrochemical Phenomena in Scanning Probe Microscopy of Ferroelectric Thin Films
journal, June 2011

Switchable Induced Polarization in LaAlO ₃ /SrTiO ₃ Heterostructures
journal, January 2012

Probing Surface and Bulk Electrochemical Processes on the LaAlO ₃ –SrTiO ₃ Interface
journal, April 2012

Probing Ferroelectrics Using Optical Second Harmonic Generation
journal, August 2011

Second harmonic generation in the lamellar ferrielectric CuInP2S6
journal, August 2000

Solid-state memories based on ferroelectric tunnel junctions
journal, December 2011

Theory of polarization of crystalline solids
journal, January 1993

Ferroelectricity at the Nanoscale: Local Polarization in Oxide Thin Films and Heterostructures
journal, April 2004

Strongly enhanced charge-density-wave order in monolayer NbSe$_2$
text, January 2015

Physics of thin-film ferroelectric oxides
text, January 2005

Room-temperature crystal structure of the layered phase CuIInIIIP2S6
journal, March 1995

Switchable Induced Polarization in LaAlO ₃ /SrTiO ₃ Heterostructures
journal, January 2012

The Role of Electrochemical Phenomena in Scanning Probe Microscopy of Ferroelectric Thin Films
journal, June 2011

Ferroelectric tunnel junctions for information storage and processing
journal, July 2014

Interface-induced nonswitchable domains in ferroelectric thin films
journal, August 2014

Flexoelectric rotation of polarization in ferroelectric thin films
journal, October 2011

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

Probing Ferroelectrics Using Optical Second Harmonic Generation
journal, August 2011

Ferroelectricity at the Nanoscale: Local Polarization in Oxide Thin Films and Heterostructures
journal, January 2004

The Piezoresponse Force Microscopy of surface layers and thin films: effective response and resolution function
text, January 2007

Physics of thin-film ferroelectric oxides
text, January 2005

Room‐Temperature Ferroelectricity in Hexagonally Layered α‐In ₂ Se ₃ Nanoflakes down to the Monolayer Limit
journal, October 2018

Metal Thio- and Selenophosphates as Multifunctional van der Waals Layered Materials
journal, August 2017

In-Plane Ferroelectricity in Thin Flakes of Van der Waals Hybrid Perovskite
journal, October 2018

Gate‐Tunable and Multidirection‐Switchable Memristive Phenomena in a Van Der Waals Ferroelectric
journal, May 2019

Spintronics of Hybrid Organic–Inorganic Perovskites: Miraculous Basis of Integrated Optoelectronic Devices
journal, June 2019

Design of Single-Molecule Multiferroics for Efficient Ultrahigh-Density Nonvolatile Memories
journal, November 2018

Recent Progress in Two‐Dimensional Ferroelectric Materials
journal, November 2019

Intrinsic Dipole Coupling in 2D van der Waals Ferroelectrics for Gate‐Controlled Switchable Rectifier
journal, November 2019

Metall‐Phosphor‐Trichalkogenide (MPCh ₃ ): von der Synthese zu aktuellen Energieanwendungen
journal, April 2019

Metal Phosphorous Trichalcogenides (MPCh ₃ ): From Synthesis to Contemporary Energy Challenges
journal, July 2019

Space‐confined microwave synthesis of ternary‐layered BiOCl crystals with high‐performance ultraviolet photodetection
journal, August 2019

Nanocrystalline Cellulose for Anisotropic Magnetoelectric Composites
journal, May 2018

Thickness‐Dependent In‐Plane Polarization and Structural Phase Transition in van der Waals Ferroelectric CuInP ₂ S ₆
journal, December 2019

The rise of two-dimensional van der Waals ferroelectrics
journal, May 2018

Progress and prospects in low-dimensional multiferroic materials
journal, January 2019

The emerging ferroic orderings in two dimensions
journal, November 2019

Quinuclidinium salt ferroelectric thin-film with duodecuple-rotational polarization-directions
journal, April 2017

Room-temperature ferroelectricity in MoTe2 down to the atomic monolayer limit
journal, April 2019

Multiferroicity in atomic van der Waals heterostructures
journal, June 2019

Van der Waals negative capacitance transistors
journal, July 2019

Tunable quadruple-well ferroelectric van der Waals crystals
journal, November 2019

Ferroelectric switching of a two-dimensional metal
journal, July 2018

Two-dimensional materials with piezoelectric and ferroelectric functionalities
journal, June 2018

Black phosphorus and its isoelectronic materials
journal, April 2019

Monolayer AgBiP ₂ Se ₆ : an atomically thin ferroelectric semiconductor with out-plane polarization
journal, January 2017

Valley polarization and ferroelectricity in a two-dimensional GaAsC ₆ monolayer
journal, January 2019

Unique physicochemical properties of two-dimensional light absorbers facilitating photocatalysis
journal, January 2018

Proton transfer ferroelectricity/multiferroicity in rutile oxyhydroxides
journal, January 2018

Room-temperature ferroelectricity and a switchable diode effect in two-dimensional α-In ₂ Se ₃ thin layers
journal, January 2018

Intrinsic multiferroicity in two-dimensional VOCl ₂ monolayers
journal, January 2019

van der Waals forces control ferroelectric–antiferroelectric ordering in CuInP ₂ S ₆ and CuBiP ₂ Se ₆ laminar materials
journal, January 2018

Anomalous polarization switching and permanent retention in a ferroelectric ionic conductor
journal, January 2020

Niobium oxide dihalides NbOX ₂ : a new family of two-dimensional van der Waals layered materials with intrinsic ferroelectricity and antiferroelectricity
journal, January 2019

Two-dimensional ferromagnetism and driven ferroelectricity in van der Waals CuCrP ₂ S ₆
journal, January 2019

Valence mediated tunable magnetism and electronic properties by ferroelectric polarization switching in 2D FeI ₂ /In ₂ Se ₃ van der Waals heterostructures
journal, January 2019

Robust two-dimensional ferroelectricity in single-layer γ-SbP and γ-SbAs
journal, January 2019

Peculiar piezoelectricity of atomically thin planar structures
journal, January 2020