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Title: Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films

Abstract

By means of normal incidence, high flux and high energy x-rays, we have obtained total scattering data for Pair Distribution Function (PDF) analysis from thin films (tf), suitable for local structure analysis. By using amorphous substrates as support for the films, the standard Rapid Acquisition PDF setup can be applied and the scattering signal from the film can be isolated from the total scattering data through subtraction of an independently measured background signal. No angular corrections to the data are needed, as would be the case for grazing incidence measurements. We illustrate the ‘tfPDF’ method through studies of as deposited (i.e. amorphous) and crystalline FeSb3 films, where the local structure analysis gives insight into the stabilization of the metastable skutterudite FeSb3 phase. The films were prepared by depositing ultra-thin alternating layers of Fe and Sb, which interdiffuse and after annealing crystallize to form the FeSb3 structure. The tfPDF data show that the amorphous precursor phase consists of corner-sharing FeSb6 octahedra with motifs highly resembling the local structure in crystalline FeSb3. Analysis of the amorphous structure allows predicting whether the final crystalline product will form the FeSb3 phase with or without excess Sb present. The study thus illustrates how analysis ofmore » the local structure in amorphous precursor films can help to understand crystallization processes of metastable phases and opens for a range of new local structure studies of thin films.« less

Authors:
 [1];  [2];  [3];  [3];  [4];  [3];  [2];  [5]
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  1. Columbia Univ., New York, NY (United States)
  2. Aarhus Univ. (Denmark)
  3. Univ. of Oregon, Eugene, OR (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
  5. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1226021
Report Number(s):
BNL-108162-2015-JA
Journal ID: ISSN 2052-2525; R&D Project: PM032; KC0202010
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
IUCrJ
Additional Journal Information:
Journal Volume: 2; Journal Issue: 5; Journal ID: ISSN 2052-2525
Publisher:
International Union of Crystallography
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Jensen, K. M.Ø., Blichfeld, A. B., Bauers, S. R., Wood, S. R., Dooryhee, E., Johnson, D. C., Iversen, B. B., and Billinge, S. Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films. United States: N. p., 2015. Web. doi:10.1107/S2052252515012221.
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Jensen, K. M.Ø., Blichfeld, A. B., Bauers, S. R., Wood, S. R., Dooryhee, E., Johnson, D. C., Iversen, B. B., & Billinge, S. Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films. United States. https://doi.org/10.1107/S2052252515012221
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Jensen, K. M.Ø., Blichfeld, A. B., Bauers, S. R., Wood, S. R., Dooryhee, E., Johnson, D. C., Iversen, B. B., and Billinge, S. Sun . "Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films". United States. https://doi.org/10.1107/S2052252515012221. https://www.osti.gov/servlets/purl/1226021.
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@article{osti_1226021,
title = {Demonstration of thin film pair distribution function analysis (tfPDF) for the study of local structure in amorphous and crystalline thin films},
author = {Jensen, K. M.Ø. and Blichfeld, A. B. and Bauers, S. R. and Wood, S. R. and Dooryhee, E. and Johnson, D. C. and Iversen, B. B. and Billinge, S.},
abstractNote = {By means of normal incidence, high flux and high energy x-rays, we have obtained total scattering data for Pair Distribution Function (PDF) analysis from thin films (tf), suitable for local structure analysis. By using amorphous substrates as support for the films, the standard Rapid Acquisition PDF setup can be applied and the scattering signal from the film can be isolated from the total scattering data through subtraction of an independently measured background signal. No angular corrections to the data are needed, as would be the case for grazing incidence measurements. We illustrate the ‘tfPDF’ method through studies of as deposited (i.e. amorphous) and crystalline FeSb3 films, where the local structure analysis gives insight into the stabilization of the metastable skutterudite FeSb3 phase. The films were prepared by depositing ultra-thin alternating layers of Fe and Sb, which interdiffuse and after annealing crystallize to form the FeSb3 structure. The tfPDF data show that the amorphous precursor phase consists of corner-sharing FeSb6 octahedra with motifs highly resembling the local structure in crystalline FeSb3. Analysis of the amorphous structure allows predicting whether the final crystalline product will form the FeSb3 phase with or without excess Sb present. The study thus illustrates how analysis of the local structure in amorphous precursor films can help to understand crystallization processes of metastable phases and opens for a range of new local structure studies of thin films.},
doi = {10.1107/S2052252515012221},
journal = {IUCrJ},
number = 5,
volume = 2,
place = {United States},
year = {Sun Jul 05 00:00:00 EDT 2015},
month = {Sun Jul 05 00:00:00 EDT 2015}
}
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https://doi.org/10.1107/S2052252515012221
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