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Title: Surface reconstructions and modified surface states in L a 1 x C a x Mn O 3

Abstract

Here, the unique functionalities present at surfaces and interfaces of complex oxides have attracted intense research in the past decade. Yet, the fundamental mechanisms underpinning functionality are often elusive, especially in doped manganites, limiting their implementation in functional electronic devices such as memristors and spin valves. Here, we present a local probe-based study on mixed-terminated La 5/8Ca 3/8MnO 3 (LCMO) films, and reveal surface metallicity in a thin film grown by pulsed-laser deposition. Using first-principles density-functional theory calculations with Hubbard correction that are more accurate to capture effects of correlation in these systems, we show that for Ca-segregated (001) LCMO surfaces the (La,Ca)O-site terminated surfaces are half metallic due to delocalized Mn- d states populating the Fermi level, whereas the MnO 2-site terminated surfaces exhibit a half-metallic or insulating character depending on the type of surface reconstruction. Computations not only explain the current measurements, but also explain other recent surface measurements on LCMO thin films, leading to a coherent picture of how the crucial link between surface segregation and Jahn-Teller couplings in the manganese oxides tune the surface electronic/magnetic structure, thereby pointing to the fine control of transport and magnetism at the conductive oxide surface independent of the bulk.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); GLOBALFOUNDRIES, Malta, NY (United States)
  3. Univ. of Aveiro, Aveiro (Portugal)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); The Univ. of Manchester, Manchester (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1489604
Alternate Identifier(s):
OSTI ID: 1480158
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 10; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Vasudevan, Rama K., Dixit, Hemant M., Tselev, Alexander, Qiao, Liang, Meyer, Tricia L., Cooper, Valentino R., Baddorf, Arthur P., Lee, Ho Nyung, Ganesh, Panchapakesan, and Kalinin, Sergei V. Surface reconstructions and modified surface states in La1–xCaxMnO3. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.104418.
Vasudevan, Rama K., Dixit, Hemant M., Tselev, Alexander, Qiao, Liang, Meyer, Tricia L., Cooper, Valentino R., Baddorf, Arthur P., Lee, Ho Nyung, Ganesh, Panchapakesan, & Kalinin, Sergei V. Surface reconstructions and modified surface states in La1–xCaxMnO3. United States. doi:10.1103/PhysRevMaterials.2.104418.
Vasudevan, Rama K., Dixit, Hemant M., Tselev, Alexander, Qiao, Liang, Meyer, Tricia L., Cooper, Valentino R., Baddorf, Arthur P., Lee, Ho Nyung, Ganesh, Panchapakesan, and Kalinin, Sergei V. Wed . "Surface reconstructions and modified surface states in La1–xCaxMnO3". United States. doi:10.1103/PhysRevMaterials.2.104418. https://www.osti.gov/servlets/purl/1489604.
@article{osti_1489604,
title = {Surface reconstructions and modified surface states in La1–xCaxMnO3},
author = {Vasudevan, Rama K. and Dixit, Hemant M. and Tselev, Alexander and Qiao, Liang and Meyer, Tricia L. and Cooper, Valentino R. and Baddorf, Arthur P. and Lee, Ho Nyung and Ganesh, Panchapakesan and Kalinin, Sergei V.},
abstractNote = {Here, the unique functionalities present at surfaces and interfaces of complex oxides have attracted intense research in the past decade. Yet, the fundamental mechanisms underpinning functionality are often elusive, especially in doped manganites, limiting their implementation in functional electronic devices such as memristors and spin valves. Here, we present a local probe-based study on mixed-terminated La5/8Ca3/8MnO3 (LCMO) films, and reveal surface metallicity in a thin film grown by pulsed-laser deposition. Using first-principles density-functional theory calculations with Hubbard correction that are more accurate to capture effects of correlation in these systems, we show that for Ca-segregated (001) LCMO surfaces the (La,Ca)O-site terminated surfaces are half metallic due to delocalized Mn-d states populating the Fermi level, whereas the MnO2-site terminated surfaces exhibit a half-metallic or insulating character depending on the type of surface reconstruction. Computations not only explain the current measurements, but also explain other recent surface measurements on LCMO thin films, leading to a coherent picture of how the crucial link between surface segregation and Jahn-Teller couplings in the manganese oxides tune the surface electronic/magnetic structure, thereby pointing to the fine control of transport and magnetism at the conductive oxide surface independent of the bulk.},
doi = {10.1103/PhysRevMaterials.2.104418},
journal = {Physical Review Materials},
issn = {2475-9953},
number = 10,
volume = 2,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
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Figures / Tables:

FIG. 1 FIG. 1: (a) Large-scale STM topography of the surface of the LCMO film. (b) Atomically resolved image of the surface, showing two distinct terminations and two different reconstructions. FFT of the white boxed regions in [(b), inset] highlights the two different lattice structures. Scale bar in inset, 4 nm−1. (c)more » Height distribution showing half-unit-cell intervals. (d) Line profile of segment “1” in (a), confirming half-unit-cell steps. Schematic view of (1 × 1) and (√2 × √2)R45° surfaces for (e) (La, Ca)O and (f) MnO2 termination. Black lines highlight the unit cell for each type of surface. Green atoms are La/Ca, red atoms are oxygen, and purple atoms are Mn.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.