Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning
Abstract
Precision synthesis of thin films requires an improved mechanistic understanding of the structural evolution of materials at the atomic scale. Atomic layer deposition (ALD) is a critical nanofabrication technique that enables fine-tuning of atomic structure and thickness as a result of its layer-by-layer growth behavior. In this study, in situ X-ray absorption spectra of the S K-edge during ALD growth of ZnS thin films on TiO2 nanoparticles were collected and analyzed. The experimental results show that both sulfide and sulfate species form during the nucleation phase of ZnS on TiO2. As film growth proceeds, the S K-edge of the in situ ZnS film converges to that of a representative ex situ ALD ZnS film. By building representative atomistic models, a high-throughput screening method was developed to determine the most probable atomic configurations as the film structure evolves. Specifically, the screening method consisted of a supervised machine learning analysis of thousands of simulated X-ray absorption near edge structure (XANES) spectra. Atomic-level insight was gained into changes in the coordination environment of surface species as they transitioned from the nucleation phase toward the crystalline ZnS phase. The experimental and computational strategies presented herein provide an example of how in situ synchrotron-based characterizationmore »
- Authors:
-
- Univ. of Michigan, Ann Arbor, MI (United States)
- Norwegian Univ. of Science and Technology (NTNU), Trondheim (Norway)
- Stanford Univ., CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); Research Council of Norway; Austrian Research Fund (FWF)
- OSTI Identifier:
- 1598269
- Grant/Contract Number:
- AC02-76SF00515; 274459; NJ3505-N20; 1727918
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 31; Journal Issue: 21; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Trejo, Orlando, Dadlani, Anup L., De La Paz, Francisco, Acharya, Shinjita, Kravec, Rob, Nordlund, Dennis, Sarangi, Ritimukta, Prinz, Fritz B., Torgersen, Jan, and Dasgupta, Neil P. Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning. United States: N. p., 2019.
Web. doi:10.1021/acs.chemmater.9b03025.
Trejo, Orlando, Dadlani, Anup L., De La Paz, Francisco, Acharya, Shinjita, Kravec, Rob, Nordlund, Dennis, Sarangi, Ritimukta, Prinz, Fritz B., Torgersen, Jan, & Dasgupta, Neil P. Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning. United States. https://doi.org/10.1021/acs.chemmater.9b03025
Trejo, Orlando, Dadlani, Anup L., De La Paz, Francisco, Acharya, Shinjita, Kravec, Rob, Nordlund, Dennis, Sarangi, Ritimukta, Prinz, Fritz B., Torgersen, Jan, and Dasgupta, Neil P. Mon .
"Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning". United States. https://doi.org/10.1021/acs.chemmater.9b03025. https://www.osti.gov/servlets/purl/1598269.
@article{osti_1598269,
title = {Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning},
author = {Trejo, Orlando and Dadlani, Anup L. and De La Paz, Francisco and Acharya, Shinjita and Kravec, Rob and Nordlund, Dennis and Sarangi, Ritimukta and Prinz, Fritz B. and Torgersen, Jan and Dasgupta, Neil P.},
abstractNote = {Precision synthesis of thin films requires an improved mechanistic understanding of the structural evolution of materials at the atomic scale. Atomic layer deposition (ALD) is a critical nanofabrication technique that enables fine-tuning of atomic structure and thickness as a result of its layer-by-layer growth behavior. In this study, in situ X-ray absorption spectra of the S K-edge during ALD growth of ZnS thin films on TiO2 nanoparticles were collected and analyzed. The experimental results show that both sulfide and sulfate species form during the nucleation phase of ZnS on TiO2. As film growth proceeds, the S K-edge of the in situ ZnS film converges to that of a representative ex situ ALD ZnS film. By building representative atomistic models, a high-throughput screening method was developed to determine the most probable atomic configurations as the film structure evolves. Specifically, the screening method consisted of a supervised machine learning analysis of thousands of simulated X-ray absorption near edge structure (XANES) spectra. Atomic-level insight was gained into changes in the coordination environment of surface species as they transitioned from the nucleation phase toward the crystalline ZnS phase. The experimental and computational strategies presented herein provide an example of how in situ synchrotron-based characterization can be leveraged using robust modeling approaches to elucidate the ordering of atoms during thin-film growth.},
doi = {10.1021/acs.chemmater.9b03025},
journal = {Chemistry of Materials},
number = 21,
volume = 31,
place = {United States},
year = {Mon Nov 04 00:00:00 EST 2019},
month = {Mon Nov 04 00:00:00 EST 2019}
}
Web of Science
Works referenced in this record:
Economic viability of thin-film tandem solar modules in the United States
journal, April 2018
- Sofia, Sarah E.; Mailoa, Jonathan P.; Weiss, Dirk N.
- Nature Energy, Vol. 3, Issue 5
Techno-economic viability of silicon-based tandem photovoltaic modules in the United States
journal, July 2018
- Yu, Zhengshan J.; Carpenter, Joe V.; Holman, Zachary C.
- Nature Energy, Vol. 3, Issue 9
The development of flexible integrated circuits based on thin-film transistors
journal, January 2018
- Myny, Kris
- Nature Electronics, Vol. 1, Issue 1
Building logical qubits in a superconducting quantum computing system
journal, January 2017
- Gambetta, Jay M.; Chow, Jerry M.; Steffen, Matthias
- npj Quantum Information, Vol. 3, Issue 1
Atomic Layer Deposition: An Overview
journal, January 2010
- George, Steven M.
- Chemical Reviews, Vol. 110, Issue 1, p. 111-131
Modeling Mechanism and Growth Reactions for New Nanofabrication Processes by Atomic Layer Deposition
journal, December 2015
- Elliott, Simon D.; Dey, Gangotri; Maimaiti, Yasheng
- Advanced Materials, Vol. 28, Issue 27
In Situ Studies on Reaction Mechanisms in Atomic Layer Deposition
journal, January 2013
- Knapas, Kjell; Ritala, Mikko
- Critical Reviews in Solid State and Materials Sciences, Vol. 38, Issue 3
Quantifying Geometric Strain at the PbS QD-TiO 2 Anode Interface and Its Effect on Electronic Structures
journal, November 2015
- Trejo, Orlando; Roelofs, Katherine E.; Xu, Shicheng
- Nano Letters, Vol. 15, Issue 12
Exploring the local electronic structure and geometric arrangement of ALD Zn(O,S) buffer layers using X-ray absorption spectroscopy
journal, January 2015
- Dadlani, Anup L.; Trejo, Orlando; Acharya, Shinjita
- Journal of Materials Chemistry C, Vol. 3, Issue 47
ALD Zn(O,S) Thin Films’ Interfacial Chemical and Structural Configuration Probed by XAS
journal, May 2016
- Dadlani, Anup L.; Acharya, Shinjita; Trejo, Orlando
- ACS Applied Materials & Interfaces, Vol. 8, Issue 23
Sulfur: not a “silent” element any more
journal, January 2006
- Jalilehvand, Farideh
- Chem. Soc. Rev., Vol. 35, Issue 12
Theoretical approaches to x-ray absorption fine structure
journal, July 2000
- Rehr, J. J.; Albers, R. C.
- Reviews of Modern Physics, Vol. 72, Issue 3
Ab initio theory and calculations of X-ray spectra
journal, July 2009
- Rehr, John J.; Kas, Joshua J.; Prange, Micah P.
- Comptes Rendus Physique, Vol. 10, Issue 6
Parameter-free calculations of X-ray spectra with FEFF9
journal, January 2010
- Rehr, John J.; Kas, Joshua J.; Vila, Fernando D.
- Physical Chemistry Chemical Physics, Vol. 12, Issue 21
High-throughput computational X-ray absorption spectroscopy
journal, July 2018
- Mathew, Kiran; Zheng, Chen; Winston, Donald
- Scientific Data, Vol. 5, Issue 1
In situ synchrotron based x-ray techniques as monitoring tools for atomic layer deposition
journal, January 2014
- Devloo-Casier, Kilian; Ludwig, Karl F.; Detavernier, Christophe
- Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 32, Issue 1
In situ synchrotron x-ray characterization of ZnO atomic layer deposition
journal, November 2010
- Fong, D. D.; Eastman, J. A.; Kim, S. K.
- Applied Physics Letters, Vol. 97, Issue 19
Evolution of Crystal Structure During the Initial Stages of ZnO Atomic Layer Deposition
journal, January 2016
- Boichot, R.; Tian, L.; Richard, M. -I.
- Chemistry of Materials, Vol. 28, Issue 2
Observing the Nucleation Phase of Atomic Layer Deposition In Situ
journal, October 2012
- Mack, James F.; Van Stockum, Philip B.; Yemane, Yonas T.
- Chemistry of Materials, Vol. 24, Issue 22
The Problem with Determining Atomic Structure at the Nanoscale
journal, April 2007
- Billinge, S. J. L.; Levin, I.
- Science, Vol. 316, Issue 5824
Supervised Machine-Learning-Based Determination of Three-Dimensional Structure of Metallic Nanoparticles
journal, October 2017
- Timoshenko, Janis; Lu, Deyu; Lin, Yuewei
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 20
Automated generation and ensemble-learned matching of X-ray absorption spectra
journal, March 2018
- Zheng, Chen; Mathew, Kiran; Chen, Chi
- npj Computational Materials, Vol. 4, Issue 1
Classification of local chemical environments from x-ray absorption spectra using supervised machine learning
journal, March 2019
- Carbone, Matthew R.; Yoo, Shinjae; Topsakal, Mehmet
- Physical Review Materials, Vol. 3, Issue 3
TiO 2 –ZnS Cascade Electron Transport Layer for Efficient Formamidinium Tin Iodide Perovskite Solar Cells
journal, November 2016
- Ke, Weijun; Stoumpos, Constantinos C.; Logsdon, Jenna Leigh
- Journal of the American Chemical Society, Vol. 138, Issue 45
Solar cells with PbS quantum dot sensitized TiO 2 –multiwalled carbon nanotube composites, sulfide-titania gel and tin sulfide coated C-fabric
journal, January 2017
- Kokal, Ramesh K.; Deepa, Melepurath; Kalluri, Ankarao
- Physical Chemistry Chemical Physics, Vol. 19, Issue 38
Performance enhancement of mesoporous TiO2-based perovskite solar cells by ZnS ultrathin-interfacial modification layer
journal, March 2018
- Shaikh, Shoyebmohamad F.; Kwon, Hyeok-Chan; Yang, Wooseok
- Journal of Alloys and Compounds, Vol. 738
Atomic layer deposition of ZnS via in situ production of H2S
journal, July 2010
- Bakke, J. R.; King, J. S.; Jung, H. J.
- Thin Solid Films, Vol. 518, Issue 19
Design of an atomic layer deposition reactor for hydrogen sulfide compatibility
journal, April 2010
- Dasgupta, Neil P.; Mack, James F.; Langston, Michael C.
- Review of Scientific Instruments, Vol. 81, Issue 4, Article No. 044102
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis
journal, February 2013
- Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav
- Computational Materials Science, Vol. 68
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011
- Momma, Koichi; Izumi, Fujio
- Journal of Applied Crystallography, Vol. 44, Issue 6
Machine learning for molecular and materials science
journal, July 2018
- Butler, Keith T.; Davies, Daniel W.; Cartwright, Hugh
- Nature, Vol. 559, Issue 7715
Bias in random forest variable importance measures: Illustrations, sources and a solution
journal, January 2007
- Strobl, Carolin; Boulesteix, Anne-Laure; Zeileis, Achim
- BMC Bioinformatics, Vol. 8, Issue 1
Polarized X-ray absorption spectroscopy and XPS of TiS3: S K- and Ti L-edge XANES and S and Ti 2p XPS
journal, June 2005
- Fleet, M. E.; Harmer, S. L.; Liu, X.
- Surface Science, Vol. 584, Issue 2-3
In Situ S K-Edge X-ray Absorption Spectroscopy for Understanding and Developing SO x Storage Catalysts
journal, October 2005
- Dathe, Hendrik; Jentys, Andreas; Lercher, Johannes A.
- The Journal of Physical Chemistry B, Vol. 109, Issue 46
Reaction of H 2 S and S 2 with Metal/Oxide Surfaces: Band-Gap Size and Chemical Reactivity
journal, June 1998
- Rodriguez, José A.; Chaturvedi, Sanjay; Kuhn, Mark
- The Journal of Physical Chemistry B, Vol. 102, Issue 28
Adsorption and interaction of H2S/SO2 on TiO2
journal, April 1999
- Yanxin, Chen; Yi, Jiang; Wenzhao, Li
- Catalysis Today, Vol. 50, Issue 1
Density Functional Theory Study of the Adsorption and Reaction of H 2 S on TiO 2 Rutile (110) and Anatase (101) Surfaces
journal, October 2009
- Huang, Wen-Fei; Chen, Hsin-Tsung; Lin, M. C.
- The Journal of Physical Chemistry C, Vol. 113, Issue 47
Investigation of the H2S poisoning process for sensing composite material based on carbon nanotubes and metal oxides
journal, November 2016
- Duan, Yichen; Pirolli, Laurent; Teplyakov, Andrew V.
- Sensors and Actuators B: Chemical, Vol. 235
The complete reaction mechanism of H 2 S desulfurization on an anatase TiO 2 (001) surface: a density functional theory investigation
journal, January 2017
- Junkaew, Anchalee; Maitarad, Phornphimon; Arróyave, Raymundo
- Catalysis Science & Technology, Vol. 7, Issue 2
Steps on anatase TiO2(101)
journal, July 2006
- Gong, Xue-Qing; Selloni, Annabella; Batzill, Matthias
- Nature Materials, Vol. 5, Issue 8
Atomic Layer Deposition of Zinc Oxide: Diethyl Zinc Reactions and Surface Saturation from First-Principles
journal, September 2016
- Weckman, Timo; Laasonen, Kari
- The Journal of Physical Chemistry C, Vol. 120, Issue 38