Unexpected precipitates in conjunction with layer-by-layer growth in Mn-enriched La2/3Sr1/3MnO3 thin films: Precipitates in Mn-enriched LSMO films

Alexandra Steffen; Artur Glavic; Thomas Gutberlet; Haile Ambaye; Jürgen Schubert; Stephan Geprägs; Juri Barthel; Stefan Mattauch; Willi Zander; Maximilian Kruth; Patrick Schöffmann; Sabine Pütter; Thomas Brückel

doi:10.1016/j.tsf.2021.138862

Unexpected precipitates in conjunction with layer-by-layer growth in Mn-enriched La_2/3Sr_1/3MnO₃ thin films: Precipitates in Mn-enriched LSMO films

Alexandra Steffen, Artur Glavic, Thomas Gutberlet, Haile Ambaye, Jürgen Schubert, Stephan Geprägs, Juri Barthel, Stefan Mattauch, Willi Zander, Maximilian Kruth, Patrick Schöffmann, Sabine Pütter, Thomas Brückel

SNS Science Support 2

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

2 Scopus citations

Abstract

In recent years, layer-by-layer heteroepitaxy has become a versatile tool for depositing novel materials not accessible in bulk form. While it is possible to control the mono layer sequence on an atomic scale with the help of sophisticated analysis techniques, not all important features of the thin film growth are detectable. We report on a detailed analysis of layer-by-layer deposited Mn-enriched La_2/3Sr_1/3MnO₃ thin films using various, complementary experimental techniques. Our results show that, contrary to the expectations from the growth parameters and initial characterization, the films did not grow as atomic planes but segregated into layers of La_2/3Sr_1/3MnO₃ with additional embedded precipitant crystals. We attribute this separation to a Volmer-Weber island-like growth of Mn₃O₄ crystals within layers of La_2/3Sr_1/3MnO₃ due to increased surface tension inhibiting La and Sr oxides from sticking to nucleated Mn₃O₄ surfaces during the growth at high temperatures.

Original language	English
Article number	138862
Journal	Thin Solid Films
Volume	735
DOIs	https://doi.org/10.1016/j.tsf.2021.138862
State	Published - Oct 1 2021

Funding

The authors thank Olaf Holderer for initial ideas and scientific input. The authors gratefully acknowledge Harald Schneider’s instrumental support at MLZ regarding the Oxide MBE and the polarized neutron reflectometers TREFF and MARIA. The authors further like to thank Alexander Weber for his work on TREFF data reduction and initial support of PNR data interpretation. Research at Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, and U.S. Department of Energy. ORNL is managed by UT-Battelle, LLC, for the U.S. Department of Energy. This work is based upon experiments performed at the MARIA instrument operated by JCNS at the Heinz Maier-Leibnitz Zentrum (MLZ), Garching, Germany. The authors thank the Neutron Optics Group at the MLZ for providing measurement time at their Bruker D8 Discover reflectometer. The authors thank Olaf Holderer for initial ideas and scientific input. The authors gratefully acknowledge Harald Schneider's instrumental support at MLZ regarding the Oxide MBE and the polarized neutron reflectometers TREFF and MARIA. The authors further like to thank Alexander Weber for his work on TREFF data reduction and initial support of PNR data interpretation. Research at Oak Ridge National Laboratory's Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, and U.S. Department of Energy. ORNL is managed by UT-Battelle, LLC, for the U.S. Department of Energy. This work is based upon experiments performed at the MARIA instrument operated by JCNS at the Heinz Maier-Leibnitz Zentrum (MLZ), Garching, Germany. The authors thank the Neutron Optics Group at the MLZ for providing measurement time at their Bruker D8 Discover reflectometer.

Funders	Funder number
Heinz Maier-Leibnitz Zentrum
MLZ
Scientific User Facilities Division
U.S. Department of Energy
Basic Energy Sciences
Oak Ridge National Laboratory

Keywords

Lanthanum strontium manganate
Molecular beam epitaxy
Nanoscale structure
Oxides
Polarized neutron reflectometry
Precipitation
Thin film

Access to Document

10.1016/j.tsf.2021.138862

Cite this

Steffen, A., Glavic, A., Gutberlet, T., Ambaye, H., Schubert, J., Geprägs, S., Barthel, J., Mattauch, S., Zander, W., Kruth, M., Schöffmann, P., Pütter, S., & Brückel, T. (2021). Unexpected precipitates in conjunction with layer-by-layer growth in Mn-enriched La_2/3Sr_1/3MnO₃ thin films: Precipitates in Mn-enriched LSMO films. Thin Solid Films, 735, Article 138862. https://doi.org/10.1016/j.tsf.2021.138862

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abstract = "In recent years, layer-by-layer heteroepitaxy has become a versatile tool for depositing novel materials not accessible in bulk form. While it is possible to control the mono layer sequence on an atomic scale with the help of sophisticated analysis techniques, not all important features of the thin film growth are detectable. We report on a detailed analysis of layer-by-layer deposited Mn-enriched La2/3Sr1/3MnO3 thin films using various, complementary experimental techniques. Our results show that, contrary to the expectations from the growth parameters and initial characterization, the films did not grow as atomic planes but segregated into layers of La2/3Sr1/3MnO3 with additional embedded precipitant crystals. We attribute this separation to a Volmer-Weber island-like growth of Mn3O4 crystals within layers of La2/3Sr1/3MnO3 due to increased surface tension inhibiting La and Sr oxides from sticking to nucleated Mn3O4 surfaces during the growth at high temperatures.",

keywords = "Lanthanum strontium manganate, Molecular beam epitaxy, Nanoscale structure, Oxides, Polarized neutron reflectometry, Precipitation, Thin film",

author = "Alexandra Steffen and Artur Glavic and Thomas Gutberlet and Haile Ambaye and J{\"u}rgen Schubert and Stephan Gepr{\"a}gs and Juri Barthel and Stefan Mattauch and Willi Zander and Maximilian Kruth and Patrick Sch{\"o}ffmann and Sabine P{\"u}tter and Thomas Br{\"u}ckel",

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Steffen, A, Glavic, A, Gutberlet, T, Ambaye, H, Schubert, J, Geprägs, S, Barthel, J, Mattauch, S, Zander, W, Kruth, M, Schöffmann, P, Pütter, S & Brückel, T 2021, 'Unexpected precipitates in conjunction with layer-by-layer growth in Mn-enriched La_2/3Sr_1/3MnO₃ thin films: Precipitates in Mn-enriched LSMO films', Thin Solid Films, vol. 735, 138862. https://doi.org/10.1016/j.tsf.2021.138862

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T2 - Precipitates in Mn-enriched LSMO films

AU - Steffen, Alexandra

AU - Glavic, Artur

AU - Gutberlet, Thomas

AU - Ambaye, Haile

AU - Schubert, Jürgen

AU - Geprägs, Stephan

AU - Barthel, Juri

AU - Mattauch, Stefan

AU - Zander, Willi

AU - Kruth, Maximilian

AU - Schöffmann, Patrick

AU - Pütter, Sabine

AU - Brückel, Thomas

PY - 2021/10/1

Y1 - 2021/10/1

N2 - In recent years, layer-by-layer heteroepitaxy has become a versatile tool for depositing novel materials not accessible in bulk form. While it is possible to control the mono layer sequence on an atomic scale with the help of sophisticated analysis techniques, not all important features of the thin film growth are detectable. We report on a detailed analysis of layer-by-layer deposited Mn-enriched La2/3Sr1/3MnO3 thin films using various, complementary experimental techniques. Our results show that, contrary to the expectations from the growth parameters and initial characterization, the films did not grow as atomic planes but segregated into layers of La2/3Sr1/3MnO3 with additional embedded precipitant crystals. We attribute this separation to a Volmer-Weber island-like growth of Mn3O4 crystals within layers of La2/3Sr1/3MnO3 due to increased surface tension inhibiting La and Sr oxides from sticking to nucleated Mn3O4 surfaces during the growth at high temperatures.

AB - In recent years, layer-by-layer heteroepitaxy has become a versatile tool for depositing novel materials not accessible in bulk form. While it is possible to control the mono layer sequence on an atomic scale with the help of sophisticated analysis techniques, not all important features of the thin film growth are detectable. We report on a detailed analysis of layer-by-layer deposited Mn-enriched La2/3Sr1/3MnO3 thin films using various, complementary experimental techniques. Our results show that, contrary to the expectations from the growth parameters and initial characterization, the films did not grow as atomic planes but segregated into layers of La2/3Sr1/3MnO3 with additional embedded precipitant crystals. We attribute this separation to a Volmer-Weber island-like growth of Mn3O4 crystals within layers of La2/3Sr1/3MnO3 due to increased surface tension inhibiting La and Sr oxides from sticking to nucleated Mn3O4 surfaces during the growth at high temperatures.

KW - Lanthanum strontium manganate

KW - Molecular beam epitaxy

KW - Nanoscale structure

KW - Oxides

KW - Polarized neutron reflectometry

KW - Precipitation

KW - Thin film

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