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Title: Femtosecond laser ablation-based mass spectrometry. An ideal tool for stoichiometric analysis of thin films

Abstract

An accurate and routinely available method for stoichiometric analysis of thin films is a desideratum of modern materials science where a material’s properties depend sensitively on elemental composition. We thoroughly investigated femtosecond laser ablation-inductively coupled plasma-mass spectrometry (fs-LA-ICP-MS) as an analytical technique for determination of the stoichiometry of thin films down to the nanometer scale. The use of femtosecond laser ablation allows for precise removal of material with high spatial and depth resolution that can be coupled to an ICP-MS to obtain elemental and isotopic information. We used molecular beam epitaxy-grown thin films of LaPd(x)Sb2 and T´-La2CuO4 to demonstrate the capacity of fs-LA-ICP-MS for stoichiometric analysis and the spatial and depth resolution of the technique. Here we demonstrate that the stoichiometric information of thin films with a thickness of ~10 nm or lower can be determined. Furthermore, our results indicate that fs-LA-ICP-MS provides precise information on the thin film-substrate interface and is able to detect the interdiffusion of cations.

Authors:
 [1];  [2];  [3];  [2];  [4]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Purdue University, West Lafayette, IN (United States). School of Nuclear Engineering.
  2. Technische Universität Darmstadt, Darmstadt (Germany). Institute for Materials Science.
  3. Purdue University, West Lafayette, IN (United States). School of Nuclear Engineering.
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA) Office of Nonproliferation and Verification Research and Development (NA-22); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
OSTI Identifier:
1212861
Report Number(s):
PNNL-SA-107263
Journal ID: ISSN 2045-2322; srep13121
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 5; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; mass spectrometry; nanoscale materials

Citation Formats

LaHaye, Nicole L., Kurian, Jose, Diwakar, Prasoon K., Alff, Lambert, and Harilal, Sivanandan S. Femtosecond laser ablation-based mass spectrometry. An ideal tool for stoichiometric analysis of thin films. United States: N. p., 2015. Web. doi:10.1038/srep13121.
LaHaye, Nicole L., Kurian, Jose, Diwakar, Prasoon K., Alff, Lambert, & Harilal, Sivanandan S. Femtosecond laser ablation-based mass spectrometry. An ideal tool for stoichiometric analysis of thin films. United States. https://doi.org/10.1038/srep13121
LaHaye, Nicole L., Kurian, Jose, Diwakar, Prasoon K., Alff, Lambert, and Harilal, Sivanandan S. Wed . "Femtosecond laser ablation-based mass spectrometry. An ideal tool for stoichiometric analysis of thin films". United States. https://doi.org/10.1038/srep13121. https://www.osti.gov/servlets/purl/1212861.
@article{osti_1212861,
title = {Femtosecond laser ablation-based mass spectrometry. An ideal tool for stoichiometric analysis of thin films},
author = {LaHaye, Nicole L. and Kurian, Jose and Diwakar, Prasoon K. and Alff, Lambert and Harilal, Sivanandan S.},
abstractNote = {An accurate and routinely available method for stoichiometric analysis of thin films is a desideratum of modern materials science where a material’s properties depend sensitively on elemental composition. We thoroughly investigated femtosecond laser ablation-inductively coupled plasma-mass spectrometry (fs-LA-ICP-MS) as an analytical technique for determination of the stoichiometry of thin films down to the nanometer scale. The use of femtosecond laser ablation allows for precise removal of material with high spatial and depth resolution that can be coupled to an ICP-MS to obtain elemental and isotopic information. We used molecular beam epitaxy-grown thin films of LaPd(x)Sb2 and T´-La2CuO4 to demonstrate the capacity of fs-LA-ICP-MS for stoichiometric analysis and the spatial and depth resolution of the technique. Here we demonstrate that the stoichiometric information of thin films with a thickness of ~10 nm or lower can be determined. Furthermore, our results indicate that fs-LA-ICP-MS provides precise information on the thin film-substrate interface and is able to detect the interdiffusion of cations.},
doi = {10.1038/srep13121},
journal = {Scientific Reports},
number = ,
volume = 5,
place = {United States},
year = {Wed Aug 19 00:00:00 EDT 2015},
month = {Wed Aug 19 00:00:00 EDT 2015}
}

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Works referenced in this record:

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Superconducting T'-La2-xCexCuO4 Films Grown by Molecular Beam Epitaxy
journal, June 2000

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A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
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Dimensionality Control of Electronic Phase Transitions in Nickel-Oxide Superlattices
journal, May 2011


Materials chemistry and thermodynamics of REBa2Cu3O7?x
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Thin films of hard cubic Zr3N4 stabilized by stress
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Materials science: Enter the oxides
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Processing, Structure, Properties, and Applications of PZT Thin Films
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Dielectric properties in heteroepitaxial Ba0.6Sr0.4TiO3 thin films: Effect of internal stresses and dislocation-type defects
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The effect of laser pulse duration on ICP-MS signal intensity, elemental fractionation, and detection limits in fs-LA-ICP-MS
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Femtosecond laser ablation: Experimental study of the repetition rate influence on inductively coupled plasma mass spectrometry performance
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Phase control in La-214 epitaxial thin films
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  • DOI: 10.1117/12.455498

Phase control of La 2 CuO 4 in thin film synthesis
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New class of T′-structure cuprate superconductors
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