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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. In conclusion, 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]
  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.
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. doi:10.1103/PhysRevB.97.054109.
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. doi:10.1103/PhysRevB.97.054109. https://www.osti.gov/servlets/purl/1425214.
@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. In conclusion, 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 = {2018},
month = {2}
}

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Cited by: 9 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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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.