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Title: The Concept of Negative Capacitance in Ionically Conductive Van der Waals Ferroelectrics

Abstract

Abstract Negative capacitance (NC) provides a path to overcome the Boltzmann limit that dictates operating voltages in transistors and, therefore, may open up a path to the challenging proposition of lowering energy consumption and waste heat in nanoelectronic integrated circuits. Typically, NC effects in ferroelectric materials are based on either stabilizing a zero‐polarization state or slowing down ferroelectric switching in order to access NC regimes of the free‐energy distribution. Here, a fundamentally different mechanism for NC, based on CuInP 2 S 6 , a van der Waals layered ferrielectric, is demonstrated. Using density functional theory and piezoresponse force microscopy, it is shown that an unusual combination of high Cu‐ion mobility and its crucial role in determining polarization magnitude and orientation (P) leads to a negative slope of the polarization versus the electric field E, dP / dE  < 0, which is a requirement for NC. This mechanism for NC is likely to occur in a wide class of materials, offering new possibilities for NC‐based devices. The nanoscale demonstration of this mechanism can be extended to the device‐level by increasing the regions of homogeneous polarization and polarization switching, for example, through strain engineering and carefully selected electric field pulses.

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [1];  [3]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  2. Vanderbilt Univ., Nashville, TN (United States); Univ. of Chinese Academy of Sciences & Inst. of Physics, Chinese Academy of Sciences, Beijing (China)
  3. Vanderbilt Univ., Nashville, TN (United States)
  4. Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Air Force Research Laboratory
OSTI Identifier:
1694376
Alternate Identifier(s):
OSTI ID: 1804539
Grant/Contract Number:  
AC05-00OR22725; FG02‐09ER46554; AC02‐05CH11231; 19RXCOR052; DE‐FG02‐09ER46554; DE‐AC02‐05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 10; Journal Issue: 39; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Neumayer, Sabine M., Tao, Lei, O'Hara, Andrew, Susner, Michael A., McGuire, Michael A., Maksymovych, Petro, Pantelides, Sokrates T., and Balke, Nina. The Concept of Negative Capacitance in Ionically Conductive Van der Waals Ferroelectrics. United States: N. p., 2020. Web. doi:10.1002/aenm.202001726.
Neumayer, Sabine M., Tao, Lei, O'Hara, Andrew, Susner, Michael A., McGuire, Michael A., Maksymovych, Petro, Pantelides, Sokrates T., & Balke, Nina. The Concept of Negative Capacitance in Ionically Conductive Van der Waals Ferroelectrics. United States. https://doi.org/10.1002/aenm.202001726
Neumayer, Sabine M., Tao, Lei, O'Hara, Andrew, Susner, Michael A., McGuire, Michael A., Maksymovych, Petro, Pantelides, Sokrates T., and Balke, Nina. Thu . "The Concept of Negative Capacitance in Ionically Conductive Van der Waals Ferroelectrics". United States. https://doi.org/10.1002/aenm.202001726. https://www.osti.gov/servlets/purl/1694376.
@article{osti_1694376,
title = {The Concept of Negative Capacitance in Ionically Conductive Van der Waals Ferroelectrics},
author = {Neumayer, Sabine M. and Tao, Lei and O'Hara, Andrew and Susner, Michael A. and McGuire, Michael A. and Maksymovych, Petro and Pantelides, Sokrates T. and Balke, Nina},
abstractNote = {Abstract Negative capacitance (NC) provides a path to overcome the Boltzmann limit that dictates operating voltages in transistors and, therefore, may open up a path to the challenging proposition of lowering energy consumption and waste heat in nanoelectronic integrated circuits. Typically, NC effects in ferroelectric materials are based on either stabilizing a zero‐polarization state or slowing down ferroelectric switching in order to access NC regimes of the free‐energy distribution. Here, a fundamentally different mechanism for NC, based on CuInP 2 S 6 , a van der Waals layered ferrielectric, is demonstrated. Using density functional theory and piezoresponse force microscopy, it is shown that an unusual combination of high Cu‐ion mobility and its crucial role in determining polarization magnitude and orientation (P) leads to a negative slope of the polarization versus the electric field E, dP / dE  < 0, which is a requirement for NC. This mechanism for NC is likely to occur in a wide class of materials, offering new possibilities for NC‐based devices. The nanoscale demonstration of this mechanism can be extended to the device‐level by increasing the regions of homogeneous polarization and polarization switching, for example, through strain engineering and carefully selected electric field pulses.},
doi = {10.1002/aenm.202001726},
journal = {Advanced Energy Materials},
number = 39,
volume = 10,
place = {United States},
year = {Thu Sep 03 00:00:00 EDT 2020},
month = {Thu Sep 03 00:00:00 EDT 2020}
}

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

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

  • Simon, A.; Ravez, J.; Maisonneuve, V.
  • Chemistry of Materials, Vol. 6, Issue 9
  • DOI: 10.1021/cm00045a016

Differentiating Ferroelectric and Nonferroelectric Electromechanical Effects with Scanning Probe Microscopy
journal, May 2015


Negative capacitance in a ferroelectric capacitor
journal, December 2014

  • Khan, Asif Islam; Chatterjee, Korok; Wang, Brian
  • Nature Materials, Vol. 14, Issue 2
  • DOI: 10.1038/nmat4148

Alternative interpretations for decreasing voltage with increasing charge in ferroelectric capacitors
journal, February 2016

  • Song, Seul Ji; Kim, Yu Jin; Park, Min Hyuk
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep20825

Projector augmented-wave method
journal, December 1994


Flexoelectric Effect in Solids
journal, July 2013


Steep-slope hysteresis-free negative capacitance MoS2 transistors
journal, December 2017


Locally Controlled Cu-Ion Transport in Layered Ferroelectric CuInP 2 S 6
journal, July 2018

  • Balke, Nina; Neumayer, Sabine M.; Brehm, John A.
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 32
  • DOI: 10.1021/acsami.8b08079

Cation–Eutectic Transition via Sublattice Melting in CuInP 2 S 6 /In 4/3 P 2 S 6 van der Waals Layered Crystals
journal, July 2017

  • Susner, Michael A.; Chyasnavichyus, Marius; Puretzky, Alexander A.
  • ACS Nano, Vol. 11, Issue 7
  • DOI: 10.1021/acsnano.7b02695

Alignment of Polarization against an Electric Field in van der Waals Ferroelectrics
journal, June 2020


Giant negative electrostriction and dielectric tunability in a van der Waals layered ferroelectric
journal, February 2019


Negative Capacitance in Organic/Ferroelectric Capacitor to Implement Steep Switching MOS Devices
journal, June 2015


Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes
journal, August 2016

  • Liu, Fucai; You, Lu; Seyler, Kyle L.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12357

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


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Steep switching devices for low power applications: negative differential capacitance/resistance field effect transistors
journal, January 2018


Pressure-induced phase transition in ferrielectric CuInP2S6
journal, August 1998


Theory of polarization of crystalline solids
journal, January 1993


Negative Capacitance in Short-Channel FinFETs Externally Connected to an Epitaxial Ferroelectric Capacitor
journal, January 2016

  • Khan, Asif Islam; Chatterjee, Korok; Duarte, Juan Pablo
  • IEEE Electron Device Letters, Vol. 37, Issue 1
  • DOI: 10.1109/LED.2015.2501319

Experimental evidence of ferroelectric negative capacitance in nanoscale heterostructures
journal, September 2011

  • Islam Khan, Asif; Bhowmik, Debanjan; Yu, Pu
  • Applied Physics Letters, Vol. 99, Issue 11
  • DOI: 10.1063/1.3634072

High- T c Layered Ferrielectric Crystals by Coherent Spinodal Decomposition
journal, October 2015


Unconventional out-of-plane domain inversion via in-plane ionic migration in a van der Waals ferroelectric
journal, January 2020

  • Xu, Dong-Dong; Ma, Ru-Ru; Zhao, Yi-Feng
  • Journal of Materials Chemistry C, Vol. 8, Issue 21
  • DOI: 10.1039/D0TC01620A

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


Macroscopic polarization in crystalline dielectrics: the geometric phase approach
journal, July 1994


Switching spectroscopy piezoresponse force microscopy of ferroelectric materials
journal, February 2006

  • Jesse, Stephen; Baddorf, Arthur P.; Kalinin, Sergei V.
  • Applied Physics Letters, Vol. 88, Issue 6
  • DOI: 10.1063/1.2172216

“Negative capacitance” in resistor-ferroelectric and ferroelectric-dielectric networks: Apparent or intrinsic?
journal, March 2018

  • Saha, Atanu K.; Datta, Suman; Gupta, Sumeet K.
  • Journal of Applied Physics, Vol. 123, Issue 10
  • DOI: 10.1063/1.5016152

On the stabilization of ferroelectric negative capacitance in nanoscale devices
journal, January 2018

  • Hoffmann, Michael; Pešić, Milan; Slesazeck, Stefan
  • Nanoscale, Vol. 10, Issue 23
  • DOI: 10.1039/C8NR02752H

Effect of the damping function in dispersion corrected density functional theory
journal, March 2011

  • Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars
  • Journal of Computational Chemistry, Vol. 32, Issue 7
  • DOI: 10.1002/jcc.21759

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

  • Zhou, Shuang; You, Lu; Chaturvedi, Apoorva
  • Materials Horizons, Vol. 7, Issue 1
  • DOI: 10.1039/C9MH01215J

Harnessing ferroelectric domains for negative capacitance
journal, February 2019


A comparison of Ag- and proton-conducting ferroelectrics
journal, October 1999


Room-Temperature Negative Capacitance in a Ferroelectric–Dielectric Superlattice Heterostructure
journal, September 2014

  • Gao, Weiwei; Khan, Asif; Marti, Xavi
  • Nano Letters, Vol. 14, Issue 10
  • DOI: 10.1021/nl502691u

Negative capacitance to the rescue?
journal, February 2008


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

  • Susner, Michael A.; Chyasnavichyus, Marius; McGuire, Michael A.
  • Advanced Materials, Vol. 29, Issue 38
  • DOI: 10.1002/adma.201602852

Spatially resolved steady-state negative capacitance
journal, January 2019


Voltage Drop in a Ferroelectric Single Layer Capacitor by Retarded Domain Nucleation
journal, November 2017


Use of Negative Capacitance to Provide Voltage Amplification for Low Power Nanoscale Devices
journal, February 2008

  • Salahuddin, Sayeef; Datta, Supriyo
  • Nano Letters, Vol. 8, Issue 2
  • DOI: 10.1021/nl071804g

Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Dielectric and ultrasonic investigation of phase transition in cuinp 2 s 6 crystals
journal, April 2004


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


A density-functional model of the dispersion interaction
journal, October 2005

  • Becke, Axel D.; Johnson, Erin R.
  • The Journal of Chemical Physics, Vol. 123, Issue 15
  • DOI: 10.1063/1.2065267

A critical review of recent progress on negative capacitance field-effect transistors
journal, March 2019

  • Alam, Muhammad A.; Si, Mengwei; Ye, Peide D.
  • Applied Physics Letters, Vol. 114, Issue 9
  • DOI: 10.1063/1.5092684

Ferroelectric negative capacitance domain dynamics
journal, May 2018

  • Hoffmann, Michael; Khan, Asif Islam; Serrao, Claudy
  • Journal of Applied Physics, Vol. 123, Issue 18
  • DOI: 10.1063/1.5030072

Ionic conductivity in ferroic CuInP 2 S 6 and CuCrP 2 S 6
journal, May 1997


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


Van der Waals negative capacitance transistors
journal, July 2019


Big data and deep data in scanning and electron microscopies: deriving functionality from multidimensional data sets
journal, May 2015

  • Belianinov, Alex; Vasudevan, Rama; Strelcov, Evgheni
  • Advanced Structural and Chemical Imaging, Vol. 1, Issue 1
  • DOI: 10.1186/s40679-015-0006-6

Quantification of surface displacements and electromechanical phenomena via dynamic atomic force microscopy
journal, September 2016


31 P MAS NMR Study of the Ferrielectric−Paraelectric Transition in Layered CuInP 2 S 6
journal, October 1999

  • Bourdon, X.; Grimmer, A. -R.; Cajipe, V. B.
  • Chemistry of Materials, Vol. 11, Issue 10
  • DOI: 10.1021/cm980776n