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Title: Real Space Visualization of Competing Phases in La0.6Sr2.4Mn2O7 Single Crystals

Abstract

Correlated quantum materials are expected to provide the foundation for the next generation of information or energy technologies. A key feature of these materials is the proximity of multiple ground states close in energy, which results in the ability to tune properties with small changes in an external parameter such as magnetic field, composition, or temperature. For example, the colossal magnetoresistance exhibited by manganites is related to charge and orbital ordering and results from a metallic ferromagnetic phase in proximity to a paramagnetic insulating phase. The presence of competing ground states, at the heart of the physics and functionality of these materials, often results in nanoscale phase separation. Probing nanoscale phase separation with conventional diffraction techniques alone is not adequate, particularly when the domains are small or nanosized. In the present work we use a scanning transmission electron microscopy image-based technique of picometer precision strain maps (PPSM) to directly visualize the competing nanoscale phases with charge and orbital ordering in a double-layer manganite. This work underscores the role of subtle structural distortions in determining the electron physics in correlated quantum materials and provides insights into designing new functionalities via spatially tuning multiple competing ground states.

Authors:
ORCiD logo [1];  [2];  [2]; ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1482431
Alternate Identifier(s):
OSTI ID: 1488565
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 21; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zheng, Qiang, Schreiber, Nathaniel J., Zheng, Hong, Yan, Jiaqiang, Mcguire, Michael A., Mitchell, J. F., Chi, Miaofang, and Sales, Brian C. Real Space Visualization of Competing Phases in La0.6Sr2.4Mn2O7 Single Crystals. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.8b03589.
Zheng, Qiang, Schreiber, Nathaniel J., Zheng, Hong, Yan, Jiaqiang, Mcguire, Michael A., Mitchell, J. F., Chi, Miaofang, & Sales, Brian C. Real Space Visualization of Competing Phases in La0.6Sr2.4Mn2O7 Single Crystals. United States. https://doi.org/10.1021/acs.chemmater.8b03589
Zheng, Qiang, Schreiber, Nathaniel J., Zheng, Hong, Yan, Jiaqiang, Mcguire, Michael A., Mitchell, J. F., Chi, Miaofang, and Sales, Brian C. Mon . "Real Space Visualization of Competing Phases in La0.6Sr2.4Mn2O7 Single Crystals". United States. https://doi.org/10.1021/acs.chemmater.8b03589. https://www.osti.gov/servlets/purl/1482431.
@article{osti_1482431,
title = {Real Space Visualization of Competing Phases in La0.6Sr2.4Mn2O7 Single Crystals},
author = {Zheng, Qiang and Schreiber, Nathaniel J. and Zheng, Hong and Yan, Jiaqiang and Mcguire, Michael A. and Mitchell, J. F. and Chi, Miaofang and Sales, Brian C.},
abstractNote = {Correlated quantum materials are expected to provide the foundation for the next generation of information or energy technologies. A key feature of these materials is the proximity of multiple ground states close in energy, which results in the ability to tune properties with small changes in an external parameter such as magnetic field, composition, or temperature. For example, the colossal magnetoresistance exhibited by manganites is related to charge and orbital ordering and results from a metallic ferromagnetic phase in proximity to a paramagnetic insulating phase. The presence of competing ground states, at the heart of the physics and functionality of these materials, often results in nanoscale phase separation. Probing nanoscale phase separation with conventional diffraction techniques alone is not adequate, particularly when the domains are small or nanosized. In the present work we use a scanning transmission electron microscopy image-based technique of picometer precision strain maps (PPSM) to directly visualize the competing nanoscale phases with charge and orbital ordering in a double-layer manganite. This work underscores the role of subtle structural distortions in determining the electron physics in correlated quantum materials and provides insights into designing new functionalities via spatially tuning multiple competing ground states.},
doi = {10.1021/acs.chemmater.8b03589},
journal = {Chemistry of Materials},
number = 21,
volume = 30,
place = {United States},
year = {Mon Oct 22 00:00:00 EDT 2018},
month = {Mon Oct 22 00:00:00 EDT 2018}
}

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Cited by: 5 works
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Figures / Tables:

Figure 1 Figure 1: Local competing and interpenetrating nanoscale domains with varying La contents in LSMO-0.7 single crystal. (a) A typical atomic-resolution HAADF-STEM image along the [001] zone axis. (b) Fast Fourier transform (FFT) pattern of (a) reveals appearance of structural modulations in this crystal. Two sets of satellite spots neighboring (000)more » and (020), corresponding to structural modulations along [110] and [1$\bar{1}$0], are arrowed green and red, respectively. The inset is the enlarged view of (000) reflection, highlighting its surrounding satellite spots. (c) A typical selected-area electron diffraction (SAED) pattern contains the similar satellite spots. The splitting of these spots indicates two modulations of different wavelength. All satellite spots in (b) were marked, and the corresponding reconstructed inverse FFT image in (d) reveals competition and interpenetration of two types of nano-scale domains, which are indicated by black and red dashed-line rectangles, respectively. The scale bar is 5 nm. (e) Average electron-energy loss spectra (EELS) for the two separated phase regions (black and red dashed-line rectangle regions, respectively) show La inhomogeneity and slight chemical shift of Mn $L$-edge. The slight difference between Mn $L$-edges while obvious difference between La $M$-edges are due to average Mn oxidation states are +3.74 and +3.67 while La/Mn atomic ratios are 0.26 and 0.33 for the two phases, respectively (see main text). Note that shift of Mn $L$-edge towards lower energy indicates lower oxidation states. Two regions also reveal different modulated periodicities, as analyzed in Figure 2 and Figure 3, respectively.« less

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