skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Combinatorial Nitrogen Gradients in Sputtered Thin Films

Abstract

High-throughput synthesis and characterization methods can significantly accelerate the rate of experimental research. For physical vapor deposition (PVD), these methods include combinatorial sputtering with intentional gradients of metal/metalloid composition, temperature, and thickness across the substrate. However, many other synthesis parameters still remain out of reach for combinatorial methods. Here, we extend combinatorial sputtering parameters to include gradients of gaseous elements in thin films. Specifically, a nitrogen gradient was generated in a thin film sample library by placing two MnTe sputtering sources with different gas flows (Ar and Ar/N2) opposite of one another during the synthesis. The nitrogen content gradient was measured along the sample surface, correlating with the distance from the nitrogen source. The phase, composition, and optoelectronic properties of the resulting thin films change as a function of the nitrogen content. Furthermore, this work shows that gradients of gaseous elements can be generated in thin films synthesized by sputtering, expanding the boundaries of combinatorial science.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5]; ORCiD logo [5];  [6]; ORCiD logo [5]
  1. Fudan Univ., Shanghai (China); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Oregon State Univ., Corvallis, OR (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  6. Fudan Univ., Shanghai (China)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1461860
Report Number(s):
NREL/JA-5K00-71391
Journal ID: ISSN 2156-8952
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Combinatorial Science
Additional Journal Information:
Journal Volume: 20; Journal Issue: 7; Journal ID: ISSN 2156-8952
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; combinatorial sputtering; thin films; nitrogen gradient

Citation Formats

Han, Yanbing, Matthews, Bethany, Roberts, Dennice, Talley, Kevin R., Bauers, Sage R., Perkins, Craig, Zhang, Qun, and Zakutayev, Andriy A.. Combinatorial Nitrogen Gradients in Sputtered Thin Films. United States: N. p., 2018. Web. https://doi.org/10.1021/acscombsci.8b00035.
Han, Yanbing, Matthews, Bethany, Roberts, Dennice, Talley, Kevin R., Bauers, Sage R., Perkins, Craig, Zhang, Qun, & Zakutayev, Andriy A.. Combinatorial Nitrogen Gradients in Sputtered Thin Films. United States. https://doi.org/10.1021/acscombsci.8b00035
Han, Yanbing, Matthews, Bethany, Roberts, Dennice, Talley, Kevin R., Bauers, Sage R., Perkins, Craig, Zhang, Qun, and Zakutayev, Andriy A.. Thu . "Combinatorial Nitrogen Gradients in Sputtered Thin Films". United States. https://doi.org/10.1021/acscombsci.8b00035. https://www.osti.gov/servlets/purl/1461860.
@article{osti_1461860,
title = {Combinatorial Nitrogen Gradients in Sputtered Thin Films},
author = {Han, Yanbing and Matthews, Bethany and Roberts, Dennice and Talley, Kevin R. and Bauers, Sage R. and Perkins, Craig and Zhang, Qun and Zakutayev, Andriy A.},
abstractNote = {High-throughput synthesis and characterization methods can significantly accelerate the rate of experimental research. For physical vapor deposition (PVD), these methods include combinatorial sputtering with intentional gradients of metal/metalloid composition, temperature, and thickness across the substrate. However, many other synthesis parameters still remain out of reach for combinatorial methods. Here, we extend combinatorial sputtering parameters to include gradients of gaseous elements in thin films. Specifically, a nitrogen gradient was generated in a thin film sample library by placing two MnTe sputtering sources with different gas flows (Ar and Ar/N2) opposite of one another during the synthesis. The nitrogen content gradient was measured along the sample surface, correlating with the distance from the nitrogen source. The phase, composition, and optoelectronic properties of the resulting thin films change as a function of the nitrogen content. Furthermore, this work shows that gradients of gaseous elements can be generated in thin films synthesized by sputtering, expanding the boundaries of combinatorial science.},
doi = {10.1021/acscombsci.8b00035},
journal = {ACS Combinatorial Science},
number = 7,
volume = 20,
place = {United States},
year = {2018},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: (a) Illustration of the combinatorial sputtering method used to create nitrogen gradient in thin film sample library. Two idnetical MnTe sputtering targets are set up opposing each other, one recieving Ar as sputtering gas, while the other one receiving both Ar and N2 through gas outlets that aremore » on the opposite of each gun shield. The square substrate is placed above, such that a thin film material library is produced. (b) A grid of 44 points on the sample is established for spatial characterization. The distance of each point between the nitrogen source decreases from top right to bottom left along the sample diagonal. The distance from the nitrogen source in this work is defined as the distance from the intersection of substrate plane and the extrapolation of the Ar+N2 gas pipe.« less

Save / Share:

Works referenced in this record:

Applications of high throughput (combinatorial) methodologies to electronic, magnetic, optical, and energy-related materials
journal, June 2013

  • Green, Martin L.; Takeuchi, Ichiro; Hattrick-Simpers, Jason R.
  • Journal of Applied Physics, Vol. 113, Issue 23
  • DOI: 10.1063/1.4803530

Fulfilling the promise of the materials genome initiative with high-throughput experimental methodologies
journal, March 2017

  • Green, M. L.; Choi, C. L.; Hattrick-Simpers, J. R.
  • Applied Physics Reviews, Vol. 4, Issue 1
  • DOI: 10.1063/1.4977487

Combinatorial and High-Throughput Screening of Materials Libraries: Review of State of the Art
journal, August 2011

  • Potyrailo, Radislav; Rajan, Krishna; Stoewe, Klaus
  • ACS Combinatorial Science, Vol. 13, Issue 6
  • DOI: 10.1021/co200007w

Optoelectronic Properties of Strontium and Barium Copper Sulfides Prepared by Combinatorial Sputtering
journal, September 2017


High-Throughput Structural and Functional Characterization of the Thin Film Materials System Ni–Co–Al
journal, August 2017

  • Decker, Peer; Naujoks, Dennis; Langenkämper, Dennis
  • ACS Combinatorial Science, Vol. 19, Issue 10
  • DOI: 10.1021/acscombsci.6b00176

Combinatorial Reactive Sputtering of In 2 S 3 as an Alternative Contact Layer for Thin Film Solar Cells
journal, May 2016

  • Siol, Sebastian; Dhakal, Tara P.; Gudavalli, Ganesh S.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 22
  • DOI: 10.1021/acsami.6b02213

Combinatorial In Situ Photoelectron Spectroscopy Investigation of Sb 2 Se 3 /ZnS Heterointerfaces
journal, November 2016

  • Siol, Sebastian; Schulz, Philip; Young, Matthew
  • Advanced Materials Interfaces, Vol. 3, Issue 24
  • DOI: 10.1002/admi.201600755

A comparative study of reactor designs for the production of graded films with applications to combinatorial CVD
journal, January 2008


Combinatorial atmospheric pressure chemical vapour deposition (cAPCVD) of a mixed vanadium oxide and vanadium oxynitride thin film
journal, January 2009

  • Kafizas, Andreas; Hyett, Geoffrey; Parkin, Ivan P.
  • Journal of Materials Chemistry, Vol. 19, Issue 10
  • DOI: 10.1039/b817429f

Deliberate and Accidental Gas-Phase Alkali Doping of Chalcogenide Semiconductors: Cu(In,Ga)Se2
journal, February 2017

  • Colombara, Diego; Berner, Ulrich; Ciccioli, Andrea
  • Scientific Reports, Vol. 7, Issue 1
  • DOI: 10.1038/srep43266

Oxygen concentration as a combinatorial parameter: The effect of continuous oxygen vacancy variation on SnO2 layer conductivity
journal, April 2018


Wafer-scale growth of VO2 thin films using a combinatorial approach
journal, October 2015

  • Zhang, Hai-Tian; Zhang, Lei; Mukherjee, Debangshu
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9475

The origin of the inhomogeneity of electrical resistivity in magnetron-sputtered indium tin oxide thin films
journal, June 1994


Analysis of relevant plasma parameters for ZnO:Al film deposition based on data from reactive and non-reactive DC magnetron sputtering
journal, September 2003


Thin film synthesis and properties of copper nitride, a metastable semiconductor
journal, January 2014

  • Caskey, Christopher M.; Richards, Ryan M.; Ginley, David S.
  • Mater. Horiz., Vol. 1, Issue 4
  • DOI: 10.1039/C4MH00049H

Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures
journal, April 2016

  • Caskey, Christopher M.; Holder, Aaron; Shulda, Sarah
  • The Journal of Chemical Physics, Vol. 144, Issue 14
  • DOI: 10.1063/1.4945561

Thin films of CuInSe 2 produced by rf sputtering with intentional oxygen doping
journal, June 1991

  • Yamaguchi, Toshiyuki; Matsufusa, Jiro; Kabasawa, Hideki
  • Journal of Applied Physics, Vol. 69, Issue 11
  • DOI: 10.1063/1.347545

Synthesis of N-Doped Graphene by Chemical Vapor Deposition and Its Electrical Properties
journal, May 2009

  • Wei, Dacheng; Liu, Yunqi; Wang, Yu
  • Nano Letters, Vol. 9, Issue 5
  • DOI: 10.1021/nl803279t

Effects of Hydrogen on Acceptor Activation in Ternary Nitride Semiconductors
journal, February 2017

  • Fioretti, Angela N.; Stokes, Adam; Young, Matthew R.
  • Advanced Electronic Materials, Vol. 3, Issue 3
  • DOI: 10.1002/aelm.201600544

Hydrogen passivation in nitrogen and chlorine‐doped ZnSe films grown by gas source molecular beam epitaxy
journal, February 1995

  • Ho, E.; Fisher, P. A.; House, J. L.
  • Applied Physics Letters, Vol. 66, Issue 9
  • DOI: 10.1063/1.113574

On the road to self-sputtering in high power impulse magnetron sputtering: particle balance and discharge characteristics
journal, April 2014


Thin films of SnO2:F by reactive magnetron sputtering with rapid thermal post-annealing
journal, February 2014


Accelerated development of CuSbS 2 thin film photovoltaic device prototypes : Accelerated development of CuSbS
journal, February 2016

  • Welch, Adam W.; Baranowski, Lauryn L.; Zawadzki, Pawel
  • Progress in Photovoltaics: Research and Applications, Vol. 24, Issue 7
  • DOI: 10.1002/pip.2735

Trade-Offs in Thin Film Solar Cells with Layered Chalcostibite Photovoltaic Absorbers
journal, January 2017

  • Welch, Adam W.; Baranowski, Lauryn L.; Peng, Haowei
  • Advanced Energy Materials, Vol. 7, Issue 11
  • DOI: 10.1002/aenm.201601935

Development and application of an instrument for spatially resolved Seebeck coefficient measurements
journal, May 2013

  • Zakutayev, Andriy; Luciano, Frank J.; Bollinger, Vincent P.
  • Review of Scientific Instruments, Vol. 84, Issue 5
  • DOI: 10.1063/1.4804634

Design of Semiconducting Tetrahedral Mn 1 x Zn x O Alloys and Their Application to Solar Water Splitting
journal, May 2015


Semiconducting properties of spinel tin nitride and other IV 3 N 4 polymorphs
journal, January 2015

  • Caskey, Christopher M.; Seabold, Jason A.; Stevanović, Vladan
  • Journal of Materials Chemistry C, Vol. 3, Issue 6
  • DOI: 10.1039/C4TC02528H

19·9%-efficient ZnO/CdS/CuInGaSe 2 solar cell with 81·2% fill factor
journal, May 2008

  • Repins, Ingrid; Contreras, Miguel A.; Egaas, Brian
  • Progress in Photovoltaics: Research and Applications, Vol. 16, Issue 3
  • DOI: 10.1002/pip.822

An open experimental database for exploring inorganic materials
journal, April 2018

  • Zakutayev, Andriy; Wunder, Nick; Schwarting, Marcus
  • Scientific Data, Vol. 5, Issue 1
  • DOI: 10.1038/sdata.2018.53

Carrier-induced ferromagnetic interactions in p-doped Zn(1−x)MnxTe epilayers
journal, June 2000


Nitrogen doping of tellurium‐based II–VI compounds during growth by molecular beam epitaxy
journal, November 1995

  • Baron, T.; Saminadayar, K.; Magnea, N.
  • Applied Physics Letters, Vol. 67, Issue 20
  • DOI: 10.1063/1.114829

Growth of p-type ZnTe thin films by using nitrogen doping during pulsed laser deposition
journal, August 2015

  • Lee, Kyoung Su; Oh, Gyujin; Kim, Eun Kyu
  • Journal of the Korean Physical Society, Vol. 67, Issue 4
  • DOI: 10.3938/jkps.67.672

    Works referencing / citing this record:

    Wurtzite materials in alloys of rock salt compounds
    journal, January 2020

    • Han, Yanbing; Millican, Samantha L.; Liu, Jun
    • Journal of Materials Research, Vol. 35, Issue 8
    • DOI: 10.1557/jmr.2019.402

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