Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions

Qinqin Wang; Ti Xie; Nicholas A. Blumenschein; Zhihao Song; Jimmy C. Kotsakidis; Aubrey T. Hanbicki; Michael A. Susner; Benjamin S. Conner; Qishuo Tan; Seng Huat Lee; Zhiqiang Mao; Xi Ling; Tony Low; Jian Ping Wang; Adam L. Friedman; Cheng Gong

doi:10.1016/j.matt.2022.10.014

Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions

Qinqin Wang, Ti Xie, Nicholas A. Blumenschein, Zhihao Song, Jimmy C. Kotsakidis, Aubrey T. Hanbicki, Michael A. Susner, Benjamin S. Conner, Qishuo Tan, Seng Huat Lee, Zhiqiang Mao, Xi Ling, Tony Low, Jian Ping Wang, Adam L. Friedman, Cheng Gong

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

9 Scopus citations

Abstract

The ability to engineer potential profiles of multilayered materials is critical for designing high-performance tunneling devices such as ferroelectric tunnel junctions (FTJs). FTJs comprise asymmetric electrodes and a ferroelectric spacer, promising semiconductor-platform-compatible logic and memory devices. However, traditional FTJs consist of metal/oxide/metal multilayered structures with unavoidable defects and interfacial trap states, which often cause compromised tunneling electroresistance (TER). Here, we constructed van der Waals (vdW) FTJs by a layered ferroelectric CuInP₂S₆ (CIPS) and graphene. Owing to the gigantic ferroelectric modulation of the chemical potentials in graphene by as large as ∼1 eV, we demonstrated a giant TER of 10⁹. While inserting just a monolayer MoS₂ between CIPS/graphene, the off state is further suppressed, leading to >10¹⁰ TER. Our discovery opens a new solid-state paradigm where potential profiles can be unprecedentedly engineered in a layer-by-layer fashion, fundamentally strengthening the ability to manipulate electrons’ tunneling behaviors and design advanced tunneling devices.

Original language	English (US)
Pages (from-to)	4425-4436
Number of pages	12
Journal	Matter
Volume	5
Issue number	12
DOIs	https://doi.org/10.1016/j.matt.2022.10.014
State	Published - Dec 7 2022

Bibliographical note

Funding Information:
C.G. acknowledges the grant support from Air Force Office of Scientific Research under the award number FA9550-22-1-0349, Naval Air Warfare Center Aircraft Division under the award number N00421-22-1-0001, and Army Research Laboratory under the cooperative agreement number W911NF-19-2-0181. J.-P.W. acknowledges the support of the Robert F. Hartmann Endowed Chair Professorship. M.A.S. and B.S.C. acknowledge support through the United States Air Force Office of Scientific Research (AFOSR) LRIR 18RQCOR100 and AOARD-MOST grant number F4GGA21207H002. B.S.C. further acknowledges the National Research Council Senior Fellowship award. Financial support for WSe2 sample preparation was provided by the National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) under National Science Foundation cooperative agreement DMR-2039351. Q.W. acknowledges DFT support from Dr. Qirui Cui. C.G. conceived and supervised the project. Q.W. T.X. and Z.S. fabricated tunneling devices and carried out the Raman characterizations under the supervision of C.G. Q.W. T.X. and N.A.B. conducted the electrical measurements with assistance from A.T.H. under the supervision of C.G. and A.L.F. J.C.K. carried out AFM measurements under the supervision of A.L.F. M.A.S. and B.S.C. synthesized CIPS crystals via a flux-based method. Q.T. and X.L. synthesized CIPS crystals via a chemical vapor transport method. S.H.L. and Z.M. synthesized WSe2 crystals. J.-P.W. and T.L. participated in the development of the device concept of vdW FTJs. Q.W. and C.G. analyzed the data. Q.W. and C.G. wrote the manuscript with assistance from Z.S. All authors commented on the manuscript. The authors declare no competing interests.

Funding Information:
C.G. acknowledges the grant support from Air Force Office of Scientific Research under the award number FA9550-22-1-0349 , Naval Air Warfare Center Aircraft Division under the award number N00421-22-1-0001 , and Army Research Laboratory under the cooperative agreement number W911NF-19-2-0181 . J.-P.W. acknowledges the support of the Robert F. Hartmann Endowed Chair Professorship. M.A.S. and B.S.C. acknowledge support through the United States Air Force Office of Scientific Research ( AFOSR ) LRIR 18RQCOR100 and AOARD- MOST grant number F4GGA21207H002 . B.S.C. further acknowledges the National Research Council Senior Fellowship award. Financial support for WSe 2 sample preparation was provided by the National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform ( 2DCC-MIP ) under National Science Foundation cooperative agreement DMR-2039351 . Q.W. acknowledges DFT support from Dr. Qirui Cui.

Publisher Copyright:
© 2022 Elsevier Inc.

Keywords

MAP2: Benchmark
ferroelectric tunnel junction
giant tunneling electroresistance
two-dimensional materials
van der Waals ferroelectrics

Publisher link

10.1016/j.matt.2022.10.014

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Wang, Q., Xie, T., Blumenschein, N. A., Song, Z., Kotsakidis, J. C., Hanbicki, A. T., Susner, M. A., Conner, B. S., Tan, Q., Lee, S. H., Mao, Z., Ling, X., Low, T., Wang, J. P., Friedman, A. L., & Gong, C. (2022). Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions. Matter, 5(12), 4425-4436. https://doi.org/10.1016/j.matt.2022.10.014

Wang, Q, Xie, T, Blumenschein, NA, Song, Z, Kotsakidis, JC, Hanbicki, AT, Susner, MA, Conner, BS, Tan, Q, Lee, SH, Mao, Z, Ling, X, Low, T , Wang, JP, Friedman, AL & Gong, C 2022, 'Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions', Matter, vol. 5, no. 12, pp. 4425-4436. https://doi.org/10.1016/j.matt.2022.10.014

@article{f417161613c14cba8924a4904af3ef02,

title = "Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions",

abstract = "The ability to engineer potential profiles of multilayered materials is critical for designing high-performance tunneling devices such as ferroelectric tunnel junctions (FTJs). FTJs comprise asymmetric electrodes and a ferroelectric spacer, promising semiconductor-platform-compatible logic and memory devices. However, traditional FTJs consist of metal/oxide/metal multilayered structures with unavoidable defects and interfacial trap states, which often cause compromised tunneling electroresistance (TER). Here, we constructed van der Waals (vdW) FTJs by a layered ferroelectric CuInP2S6 (CIPS) and graphene. Owing to the gigantic ferroelectric modulation of the chemical potentials in graphene by as large as ∼1 eV, we demonstrated a giant TER of 109. While inserting just a monolayer MoS2 between CIPS/graphene, the off state is further suppressed, leading to >1010 TER. Our discovery opens a new solid-state paradigm where potential profiles can be unprecedentedly engineered in a layer-by-layer fashion, fundamentally strengthening the ability to manipulate electrons{\textquoteright} tunneling behaviors and design advanced tunneling devices.",

keywords = "MAP2: Benchmark, ferroelectric tunnel junction, giant tunneling electroresistance, two-dimensional materials, van der Waals ferroelectrics",

author = "Qinqin Wang and Ti Xie and Blumenschein, {Nicholas A.} and Zhihao Song and Kotsakidis, {Jimmy C.} and Hanbicki, {Aubrey T.} and Susner, {Michael A.} and Conner, {Benjamin S.} and Qishuo Tan and Lee, {Seng Huat} and Zhiqiang Mao and Xi Ling and Tony Low and Wang, {Jian Ping} and Friedman, {Adam L.} and Cheng Gong",

note = "Funding Information: C.G. acknowledges the grant support from Air Force Office of Scientific Research under the award number FA9550-22-1-0349, Naval Air Warfare Center Aircraft Division under the award number N00421-22-1-0001, and Army Research Laboratory under the cooperative agreement number W911NF-19-2-0181. J.-P.W. acknowledges the support of the Robert F. Hartmann Endowed Chair Professorship. M.A.S. and B.S.C. acknowledge support through the United States Air Force Office of Scientific Research (AFOSR) LRIR 18RQCOR100 and AOARD-MOST grant number F4GGA21207H002. B.S.C. further acknowledges the National Research Council Senior Fellowship award. Financial support for WSe2 sample preparation was provided by the National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) under National Science Foundation cooperative agreement DMR-2039351. Q.W. acknowledges DFT support from Dr. Qirui Cui. C.G. conceived and supervised the project. Q.W. T.X. and Z.S. fabricated tunneling devices and carried out the Raman characterizations under the supervision of C.G. Q.W. T.X. and N.A.B. conducted the electrical measurements with assistance from A.T.H. under the supervision of C.G. and A.L.F. J.C.K. carried out AFM measurements under the supervision of A.L.F. M.A.S. and B.S.C. synthesized CIPS crystals via a flux-based method. Q.T. and X.L. synthesized CIPS crystals via a chemical vapor transport method. S.H.L. and Z.M. synthesized WSe2 crystals. J.-P.W. and T.L. participated in the development of the device concept of vdW FTJs. Q.W. and C.G. analyzed the data. Q.W. and C.G. wrote the manuscript with assistance from Z.S. All authors commented on the manuscript. The authors declare no competing interests. Funding Information: C.G. acknowledges the grant support from Air Force Office of Scientific Research under the award number FA9550-22-1-0349 , Naval Air Warfare Center Aircraft Division under the award number N00421-22-1-0001 , and Army Research Laboratory under the cooperative agreement number W911NF-19-2-0181 . J.-P.W. acknowledges the support of the Robert F. Hartmann Endowed Chair Professorship. M.A.S. and B.S.C. acknowledge support through the United States Air Force Office of Scientific Research ( AFOSR ) LRIR 18RQCOR100 and AOARD- MOST grant number F4GGA21207H002 . B.S.C. further acknowledges the National Research Council Senior Fellowship award. Financial support for WSe 2 sample preparation was provided by the National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform ( 2DCC-MIP ) under National Science Foundation cooperative agreement DMR-2039351 . Q.W. acknowledges DFT support from Dr. Qirui Cui. Publisher Copyright: {\textcopyright} 2022 Elsevier Inc.",

year = "2022",

month = dec,

day = "7",

doi = "10.1016/j.matt.2022.10.014",

language = "English (US)",

volume = "5",

pages = "4425--4436",

journal = "Matter",

issn = "2590-2393",

publisher = "Cell Press",

number = "12",

}

TY - JOUR

T1 - Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions

AU - Wang, Qinqin

AU - Xie, Ti

AU - Blumenschein, Nicholas A.

AU - Song, Zhihao

AU - Kotsakidis, Jimmy C.

AU - Hanbicki, Aubrey T.

AU - Susner, Michael A.

AU - Conner, Benjamin S.

AU - Tan, Qishuo

AU - Lee, Seng Huat

AU - Mao, Zhiqiang

AU - Ling, Xi

AU - Low, Tony

AU - Wang, Jian Ping

AU - Friedman, Adam L.

AU - Gong, Cheng

N1 - Funding Information: C.G. acknowledges the grant support from Air Force Office of Scientific Research under the award number FA9550-22-1-0349, Naval Air Warfare Center Aircraft Division under the award number N00421-22-1-0001, and Army Research Laboratory under the cooperative agreement number W911NF-19-2-0181. J.-P.W. acknowledges the support of the Robert F. Hartmann Endowed Chair Professorship. M.A.S. and B.S.C. acknowledge support through the United States Air Force Office of Scientific Research (AFOSR) LRIR 18RQCOR100 and AOARD-MOST grant number F4GGA21207H002. B.S.C. further acknowledges the National Research Council Senior Fellowship award. Financial support for WSe2 sample preparation was provided by the National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) under National Science Foundation cooperative agreement DMR-2039351. Q.W. acknowledges DFT support from Dr. Qirui Cui. C.G. conceived and supervised the project. Q.W. T.X. and Z.S. fabricated tunneling devices and carried out the Raman characterizations under the supervision of C.G. Q.W. T.X. and N.A.B. conducted the electrical measurements with assistance from A.T.H. under the supervision of C.G. and A.L.F. J.C.K. carried out AFM measurements under the supervision of A.L.F. M.A.S. and B.S.C. synthesized CIPS crystals via a flux-based method. Q.T. and X.L. synthesized CIPS crystals via a chemical vapor transport method. S.H.L. and Z.M. synthesized WSe2 crystals. J.-P.W. and T.L. participated in the development of the device concept of vdW FTJs. Q.W. and C.G. analyzed the data. Q.W. and C.G. wrote the manuscript with assistance from Z.S. All authors commented on the manuscript. The authors declare no competing interests. Funding Information: C.G. acknowledges the grant support from Air Force Office of Scientific Research under the award number FA9550-22-1-0349 , Naval Air Warfare Center Aircraft Division under the award number N00421-22-1-0001 , and Army Research Laboratory under the cooperative agreement number W911NF-19-2-0181 . J.-P.W. acknowledges the support of the Robert F. Hartmann Endowed Chair Professorship. M.A.S. and B.S.C. acknowledge support through the United States Air Force Office of Scientific Research ( AFOSR ) LRIR 18RQCOR100 and AOARD- MOST grant number F4GGA21207H002 . B.S.C. further acknowledges the National Research Council Senior Fellowship award. Financial support for WSe 2 sample preparation was provided by the National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform ( 2DCC-MIP ) under National Science Foundation cooperative agreement DMR-2039351 . Q.W. acknowledges DFT support from Dr. Qirui Cui. Publisher Copyright: © 2022 Elsevier Inc.

PY - 2022/12/7

Y1 - 2022/12/7

N2 - The ability to engineer potential profiles of multilayered materials is critical for designing high-performance tunneling devices such as ferroelectric tunnel junctions (FTJs). FTJs comprise asymmetric electrodes and a ferroelectric spacer, promising semiconductor-platform-compatible logic and memory devices. However, traditional FTJs consist of metal/oxide/metal multilayered structures with unavoidable defects and interfacial trap states, which often cause compromised tunneling electroresistance (TER). Here, we constructed van der Waals (vdW) FTJs by a layered ferroelectric CuInP2S6 (CIPS) and graphene. Owing to the gigantic ferroelectric modulation of the chemical potentials in graphene by as large as ∼1 eV, we demonstrated a giant TER of 109. While inserting just a monolayer MoS2 between CIPS/graphene, the off state is further suppressed, leading to >1010 TER. Our discovery opens a new solid-state paradigm where potential profiles can be unprecedentedly engineered in a layer-by-layer fashion, fundamentally strengthening the ability to manipulate electrons’ tunneling behaviors and design advanced tunneling devices.

AB - The ability to engineer potential profiles of multilayered materials is critical for designing high-performance tunneling devices such as ferroelectric tunnel junctions (FTJs). FTJs comprise asymmetric electrodes and a ferroelectric spacer, promising semiconductor-platform-compatible logic and memory devices. However, traditional FTJs consist of metal/oxide/metal multilayered structures with unavoidable defects and interfacial trap states, which often cause compromised tunneling electroresistance (TER). Here, we constructed van der Waals (vdW) FTJs by a layered ferroelectric CuInP2S6 (CIPS) and graphene. Owing to the gigantic ferroelectric modulation of the chemical potentials in graphene by as large as ∼1 eV, we demonstrated a giant TER of 109. While inserting just a monolayer MoS2 between CIPS/graphene, the off state is further suppressed, leading to >1010 TER. Our discovery opens a new solid-state paradigm where potential profiles can be unprecedentedly engineered in a layer-by-layer fashion, fundamentally strengthening the ability to manipulate electrons’ tunneling behaviors and design advanced tunneling devices.

KW - MAP2: Benchmark

KW - ferroelectric tunnel junction

KW - giant tunneling electroresistance

KW - two-dimensional materials

KW - van der Waals ferroelectrics

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JO - Matter

JF - Matter

IS - 12

ER -

Extraordinary tunnel electroresistance in layer-by-layer engineered van der Waals ferroelectric tunnel junctions

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