Surface Chemistry Controls Anomalous Ferroelectric Behavior in Lithium Niobate

Sabine M. Neumayer; Anton V. Ievlev; Liam Collins; Rama Vasudevan; Mohammad A. Baghban; Olga Ovchinnikova; Stephen Jesse; Katia Gallo; Brian J. Rodriguez; Sergei V. Kalinin

doi:10.1021/acsami.8b09513

Surface Chemistry Controls Anomalous Ferroelectric Behavior in Lithium Niobate

Sabine M. Neumayer, Anton V. Ievlev, Liam Collins, Rama Vasudevan, Mohammad A. Baghban, Olga Ovchinnikova, Stephen Jesse, Katia Gallo, Brian J. Rodriguez, Sergei V. Kalinin

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

21 Scopus citations

Abstract

Polarization switching in ferroelectric materials underpins a multitude of applications ranging from nonvolatile memories to data storage to ferroelectric lithography. While traditionally considered to be a functionality of the material only, basic theoretical considerations suggest that switching is expected to be intrinsically linked to changes in the electrochemical state of the surface. Hence, the properties and dynamics of the screening charges can affect or control the switching dynamics. Despite being recognized for over 50 years, analysis of these phenomena remained largely speculative. Here, we explore polarization switching on the prototypical LiNbO₃ surface using the combination of contact mode Kelvin probe force microscopy and chemical imaging by time-of-flight mass-spectrometry and demonstrate pronounced chemical differences between the domains. These studies provide a consistent explanation to the anomalous polarization and surface charge behavior observed in LiNbO₃ and point to new opportunities in chemical control of polarization dynamics in thin films and crystals via control of surface chemistry, complementing traditional routes via bulk doping, and substrate-induced strain and tilt systems.

Original language	English
Pages (from-to)	29153-29160
Number of pages	8
Journal	ACS Applied Materials and Interfaces
Volume	10
Issue number	34
DOIs	https://doi.org/10.1021/acsami.8b09513
State	Published - Aug 29 2018

Funding

Scanning probe microscopy was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility and using instrumentation (ToF-SIMS) within ORNL’s Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The scanning probe microscopy part of this work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences and Materials Sciences and Engineering Division (R.K.V., S.V.K., and S.M.N.). This work has in part emanated from research supported by a research grant from Science Foundation Ireland (SFI) under the US-Ireland R&D Partnership Programme grant number SFI/14/US/I3113 (S.M.N., B.J.R.). Data analysis was partially performed using pycroscopy (https://pycroscopy.github.io/pycroscopy/). Scanning probe microscopy was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility and using instrumentation (ToF-SIMS) within ORNL's Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The scanning probe microscopy part of this work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences and Materials Sciences and Engineering Division (R.K.V., S.V.K., and S.M.N.). This work has in part emanated from research supported by a research grant from Science Foundation Ireland (SFI) under the US-Ireland R&D Partnership Programme grant number SFI/14/US/I3113 (S.M.N., B.J.R.). Data analysis was partially performed using pycroscopy (https://pycroscopy.github.io/pycroscopy/).

Keywords

ferroelectrics
lithium niobate
scanning probe microscopy
surface chemistry
switching dynamics
time-of-flight secondary ion mass spectrometry

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10.1021/acsami.8b09513

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title = "Surface Chemistry Controls Anomalous Ferroelectric Behavior in Lithium Niobate",

abstract = "Polarization switching in ferroelectric materials underpins a multitude of applications ranging from nonvolatile memories to data storage to ferroelectric lithography. While traditionally considered to be a functionality of the material only, basic theoretical considerations suggest that switching is expected to be intrinsically linked to changes in the electrochemical state of the surface. Hence, the properties and dynamics of the screening charges can affect or control the switching dynamics. Despite being recognized for over 50 years, analysis of these phenomena remained largely speculative. Here, we explore polarization switching on the prototypical LiNbO3 surface using the combination of contact mode Kelvin probe force microscopy and chemical imaging by time-of-flight mass-spectrometry and demonstrate pronounced chemical differences between the domains. These studies provide a consistent explanation to the anomalous polarization and surface charge behavior observed in LiNbO3 and point to new opportunities in chemical control of polarization dynamics in thin films and crystals via control of surface chemistry, complementing traditional routes via bulk doping, and substrate-induced strain and tilt systems.",

keywords = "ferroelectrics, lithium niobate, scanning probe microscopy, surface chemistry, switching dynamics, time-of-flight secondary ion mass spectrometry",

author = "Neumayer, {Sabine M.} and Ievlev, {Anton V.} and Liam Collins and Rama Vasudevan and Baghban, {Mohammad A.} and Olga Ovchinnikova and Stephen Jesse and Katia Gallo and Rodriguez, {Brian J.} and Kalinin, {Sergei V.}",

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doi = "10.1021/acsami.8b09513",

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AU - Ievlev, Anton V.

AU - Collins, Liam

AU - Vasudevan, Rama

AU - Baghban, Mohammad A.

AU - Ovchinnikova, Olga

AU - Jesse, Stephen

AU - Gallo, Katia

AU - Rodriguez, Brian J.

AU - Kalinin, Sergei V.

PY - 2018/8/29

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N2 - Polarization switching in ferroelectric materials underpins a multitude of applications ranging from nonvolatile memories to data storage to ferroelectric lithography. While traditionally considered to be a functionality of the material only, basic theoretical considerations suggest that switching is expected to be intrinsically linked to changes in the electrochemical state of the surface. Hence, the properties and dynamics of the screening charges can affect or control the switching dynamics. Despite being recognized for over 50 years, analysis of these phenomena remained largely speculative. Here, we explore polarization switching on the prototypical LiNbO3 surface using the combination of contact mode Kelvin probe force microscopy and chemical imaging by time-of-flight mass-spectrometry and demonstrate pronounced chemical differences between the domains. These studies provide a consistent explanation to the anomalous polarization and surface charge behavior observed in LiNbO3 and point to new opportunities in chemical control of polarization dynamics in thin films and crystals via control of surface chemistry, complementing traditional routes via bulk doping, and substrate-induced strain and tilt systems.

AB - Polarization switching in ferroelectric materials underpins a multitude of applications ranging from nonvolatile memories to data storage to ferroelectric lithography. While traditionally considered to be a functionality of the material only, basic theoretical considerations suggest that switching is expected to be intrinsically linked to changes in the electrochemical state of the surface. Hence, the properties and dynamics of the screening charges can affect or control the switching dynamics. Despite being recognized for over 50 years, analysis of these phenomena remained largely speculative. Here, we explore polarization switching on the prototypical LiNbO3 surface using the combination of contact mode Kelvin probe force microscopy and chemical imaging by time-of-flight mass-spectrometry and demonstrate pronounced chemical differences between the domains. These studies provide a consistent explanation to the anomalous polarization and surface charge behavior observed in LiNbO3 and point to new opportunities in chemical control of polarization dynamics in thin films and crystals via control of surface chemistry, complementing traditional routes via bulk doping, and substrate-induced strain and tilt systems.

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KW - lithium niobate

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KW - time-of-flight secondary ion mass spectrometry

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Surface Chemistry Controls Anomalous Ferroelectric Behavior in Lithium Niobate

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