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Title: Room-temperature relaxor ferroelectricity and photovoltaic effects in tin titanate directly deposited on a silicon substrate

Abstract

Tin titanate (SnTiO3) has been notoriously impossible to prepare as a thin-film ferroelectric, probably because high-temperature annealing converts much of the Sn2+ to Sn4+. In the present paper, we show two things: first, perovskite phase SnTiO3 can be prepared by atomic-layer deposition directly onto p-type Si substrates; and second, these films exhibit ferroelectric switching at room temperature, with p-type Si acting as electrodes. X-ray diffraction measurements reveal that the film is single-phase, preferred-orientation ferroelectric perovskite SnTiO3. Our films showed well-saturated, square, and repeatable hysteresis loops of around 3μC/cm2 remnant polarization at room temperature, as detected by out-of-plane polarization versus electric field and field cycling measurements. Furthermore, photovoltaic and photoferroelectricity were found in Pt/SnTiO3/Si/SnTiO3/Pt heterostructures, the properties of which can be tuned through band-gap engineering by strain according to first-principles calculations. This is a lead-free room-temperature ferroelectric oxide of potential device application.

Authors:
 [1];  [2];  [3];  [4];  [5];  [4];  [6];  [5];  [7];  [7];  [8];  [1];  [9]
+ Show Author Affiliations
  1. Univ. of Puerto Rico, San Juan, PR (United States). Dept. of Physics and Inst. for Functional Nanomaterials
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Illinois, Chicago, IL (United States). Dept. of Chemical Engineering
  4. Univ. of Connecticut, Storrs, CT (United States). Inst. of Materials Science, Dept. of Materials Science and Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Univ. of Illinois, Chicago, IL (United States). Dept. of Chemical Engineering, and Dept. of Bioengineering
  7. Univ. of St. Andrews, Scotland (United Kingdom). School of Chemistry
  8. Univ. of St. Andrews, Scotland (United Kingdom). School of Physics and Astronomy
  9. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOD; National Research Foundation of Korea (NRF); USDOE
OSTI Identifier:
1425214
Alternate Identifier(s):
OSTI ID: 1421879; OSTI ID: 1435330
Grant/Contract Number:  
AC02-06CH11357; FA95501610295; 1002410; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 97; Journal Issue: 5; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Ferroelectricity; band-gap; density of states

Citation Formats

Agarwal, Radhe, Sharma, Yogesh, Chang, Siliang, Pitike, Krishna C., Sohn, Changhee, Nakhmanson, Serge M., Takoudis, Christos G., Lee, Ho Nyung, Tonelli, Rachel, Gardner, Jonathan, Scott, James F., Katiyar, Ram S., and Hong, Seungbum. Room-temperature relaxor ferroelectricity and photovoltaic effects in tin titanate directly deposited on a silicon substrate. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.054109.
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Agarwal, Radhe, Sharma, Yogesh, Chang, Siliang, Pitike, Krishna C., Sohn, Changhee, Nakhmanson, Serge M., Takoudis, Christos G., Lee, Ho Nyung, Tonelli, Rachel, Gardner, Jonathan, Scott, James F., Katiyar, Ram S., & Hong, Seungbum. Room-temperature relaxor ferroelectricity and photovoltaic effects in tin titanate directly deposited on a silicon substrate. United States. https://doi.org/10.1103/PhysRevB.97.054109
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Agarwal, Radhe, Sharma, Yogesh, Chang, Siliang, Pitike, Krishna C., Sohn, Changhee, Nakhmanson, Serge M., Takoudis, Christos G., Lee, Ho Nyung, Tonelli, Rachel, Gardner, Jonathan, Scott, James F., Katiyar, Ram S., and Hong, Seungbum. Tue . "Room-temperature relaxor ferroelectricity and photovoltaic effects in tin titanate directly deposited on a silicon substrate". United States. https://doi.org/10.1103/PhysRevB.97.054109. https://www.osti.gov/servlets/purl/1425214.
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@article{osti_1425214,
title = {Room-temperature relaxor ferroelectricity and photovoltaic effects in tin titanate directly deposited on a silicon substrate},
author = {Agarwal, Radhe and Sharma, Yogesh and Chang, Siliang and Pitike, Krishna C. and Sohn, Changhee and Nakhmanson, Serge M. and Takoudis, Christos G. and Lee, Ho Nyung and Tonelli, Rachel and Gardner, Jonathan and Scott, James F. and Katiyar, Ram S. and Hong, Seungbum},
abstractNote = {Tin titanate (SnTiO3) has been notoriously impossible to prepare as a thin-film ferroelectric, probably because high-temperature annealing converts much of the Sn2+ to Sn4+. In the present paper, we show two things: first, perovskite phase SnTiO3 can be prepared by atomic-layer deposition directly onto p-type Si substrates; and second, these films exhibit ferroelectric switching at room temperature, with p-type Si acting as electrodes. X-ray diffraction measurements reveal that the film is single-phase, preferred-orientation ferroelectric perovskite SnTiO3. Our films showed well-saturated, square, and repeatable hysteresis loops of around 3μC/cm2 remnant polarization at room temperature, as detected by out-of-plane polarization versus electric field and field cycling measurements. Furthermore, photovoltaic and photoferroelectricity were found in Pt/SnTiO3/Si/SnTiO3/Pt heterostructures, the properties of which can be tuned through band-gap engineering by strain according to first-principles calculations. This is a lead-free room-temperature ferroelectric oxide of potential device application.},
doi = {10.1103/PhysRevB.97.054109},
journal = {Physical Review B},
number = 5,
volume = 97,
place = {United States},
year = {Tue Feb 20 00:00:00 EST 2018},
month = {Tue Feb 20 00:00:00 EST 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/PhysRevB.97.054109
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Cited by: 27 works
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Figures / Tables:

Figure 1 Figure 1: (a) Polarization-electric field (P-E) hysteresis loop and switching current at different applied voltages between 1 and 10 V measured at room temperature. Inset shows the direction of hysteresis loop as a function of time. (b) Schematic diagram of Pt/SnTiO3/p-Si/SnTiO3/Pt capacitor structure used for electrical measurements. (c) Frequency dependencemore » of P-E hysteresis loops.« less
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Works referenced in this record:

New Type of First-Order Phase Transition in Ferroelectric Thin Films
journal, February 1973

Projector augmented-wave method
journal, December 1994

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Photoelectric Effects in Single Domain BiFeO 3 Crystals
journal, July 2012

  • Moubah, Reda; Rousseau, Olivier; Colson, Dorothée
  • Advanced Functional Materials, Vol. 22, Issue 22
  • DOI: 10.1002/adfm.201201150

Critical exponents of the dielectric constants in diffused-phase-transition crystals
journal, January 1982

Switchable photovoltaic and polarization modulated rectification in Si-integrated Pt/(Bi0.9Sm0.1)(Fe0.97Hf0.03)O3/LaNiO3 heterostructures
journal, October 2015

  • Agarwal, Radhe; Sharma, Yogesh; Katiyar, Ram S.
  • Applied Physics Letters, Vol. 107, Issue 16
  • DOI: 10.1063/1.4934665

Structural and Dielectric Properties of SnTiO 3 , a Putative Ferroelectric
journal, May 2011

  • Fix, Thomas; Sahonta, S. -Lata; Garcia, Vincent
  • Crystal Growth & Design, Vol. 11, Issue 5
  • DOI: 10.1021/cg200333q

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

Depolarization corrections to the coercive field in thin-film ferroelectrics
journal, June 2003

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

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

Photo-induced ferroelectric switching in perovskite CH 3 NH 3 PbI 3 films
journal, January 2017

  • Wang, Peiqi; Zhao, Jinjin; Wei, Liyu
  • Nanoscale, Vol. 9, Issue 11
  • DOI: 10.1039/C6NR09310H

Explanation of the apparent sublinear photoconductivity of photorefractive barium titanate
journal, April 1990

A photoferroelectric material is more than the sum of its parts
journal, March 2012

  • Kreisel, J.; Alexe, M.; Thomas, P. A.
  • Nature Materials, Vol. 11, Issue 4
  • DOI: 10.1038/nmat3282

Inhomogeneous Electron Gas
journal, November 1964

Oxygen vacancy migration and time-dependent leakage current behavior of Ba0.3Sr0.7TiO3 thin films
journal, March 2005

  • Meyer, R.; Liedtke, R.; Waser, R.
  • Applied Physics Letters, Vol. 86, Issue 11
  • DOI: 10.1063/1.1874313

Structural, Electronic, and Lattice Dynamics of PbTiO 3 , SnTiO 3 , and SnZrO 3 : A Comparative First-Principles Study
journal, January 2013

Photoferroelectric and Photopiezoelectric Properties of Organometal Halide Perovskites
journal, April 2016

Direct observation of region by region suppression of the switchable polarization (fatigue) in Pb(Zr,Ti)O3 thin film capacitors with Pt electrodes
journal, May 1998

  • Colla, E. L.; Hong, Seungbum; Taylor, D. V.
  • Applied Physics Letters, Vol. 72, Issue 21
  • DOI: 10.1063/1.121083

Unipolar resistive switching behavior of amorphous YCrO 3 films for nonvolatile memory applications
journal, August 2014

  • Sharma, Yogesh; Misra, Pankaj; Katiyar, Ram S.
  • Journal of Applied Physics, Vol. 116, Issue 8
  • DOI: 10.1063/1.4893661

Atomic layer deposition of environmentally benign SnTiO x as a potential ferroelectric material
journal, January 2016

  • Chang, Siliang; Selvaraj, Sathees Kannan; Choi, Yoon-Young
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 34, Issue 1
  • DOI: 10.1116/1.4935650

There’s no place like Ohm: conduction in oxide thin films
journal, March 2014

Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981

First-Principles Study of Lead-Free Piezoelectric SnTiO 3
journal, September 2008

  • Uratani, Yoshitaka; Shishidou, Tatsuya; Oguchi, Tamio
  • Japanese Journal of Applied Physics, Vol. 47, Issue 9
  • DOI: 10.1143/JJAP.47.7735

Ferroelectric-like hysteresis loop in nonferroelectric systems
journal, September 2005

  • Pintilie, L.; Alexe, M.
  • Applied Physics Letters, Vol. 87, Issue 11
  • DOI: 10.1063/1.2045543

First-principles study of misfit strain-stabilized ferroelectric SnTiO 3
journal, December 2011

  • Parker, William D.; Rondinelli, James M.; Nakhmanson, S. M.
  • Physical Review B, Vol. 84, Issue 24
  • DOI: 10.1103/PhysRevB.84.245126

Polarization reversal and capacitance-voltage characteristic of epitaxial Pb(Zr,Ti)O3 layers
journal, May 2005

  • Pintilie, L.; Lisca, M.; Alexe, M.
  • Applied Physics Letters, Vol. 86, Issue 19
  • DOI: 10.1063/1.1926403

Capacitance-voltage modeling of metal-ferroelectric-semiconductor capacitors based on epitaxial oxide heterostructures
journal, March 2011

  • Choi, Woong; Kim, Sunkook; Jin, Yong Wan
  • Applied Physics Letters, Vol. 98, Issue 10
  • DOI: 10.1063/1.3561751

Tip-enhanced photovoltaic effects in bismuth ferrite
journal, March 2011

  • Alexe, Marin; Hesse, Dietrich
  • Nature Communications, Vol. 2, Issue 1
  • DOI: 10.1038/ncomms1261

First principles studies of SnTiO3 perovskite as potential environmentally benign ferroelectric material
journal, January 2009

On measurement of optical band gap of chromium oxide films containing both amorphous and crystalline phases
journal, December 1997

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Screening mechanisms at polar oxide heterointerfaces
journal, June 2016

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    Tin titanate—the hunt for a new ferroelectric perovskite
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    • Gardner, J.; Thakre, Atul; Kumar, Ashok
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