Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning

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.

doi:10.1021/acs.chemmater.9b03025

Title: Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning

Journal Article · Mon Nov 04 00:00:00 EST 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b03025· OSTI ID:1598269

Trejo, Orlando ^[1]; Dadlani, Anup L. ^[2]; De La Paz, Francisco ^[3]; Acharya, Shinjita ^[3]; Kravec, Rob ^[3]; Nordlund, Dennis ^[4];

^[4]; Prinz, Fritz B. ^[3];

^[2];

^[1]

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)

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); Research Council of Norway; Austrian Research Fund (FWF)

Grant/Contract Number:: AC02-76SF00515; 274459; NJ3505-N20; 1727918

OSTI ID:: 1598269

Journal Information:: Chemistry of Materials, Vol. 31, Issue 21; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 15 works

Citation information provided by
Web of Science

References (42)

Economic viability of thin-film tandem solar modules in the United States Sofia, Sarah E.; Mailoa, Jonathan P.; Weiss, Dirk N. Nature Energy, Vol. 3, Issue 5 https://doi.org/10.1038/s41560-018-0126-z	journal	April 2018
Techno-economic viability of silicon-based tandem photovoltaic modules in the United States Yu, Zhengshan J.; Carpenter, Joe V.; Holman, Zachary C. Nature Energy, Vol. 3, Issue 9 https://doi.org/10.1038/s41560-018-0201-5	journal	July 2018
The development of flexible integrated circuits based on thin-film transistors Myny, Kris Nature Electronics, Vol. 1, Issue 1 https://doi.org/10.1038/s41928-017-0008-6	journal	January 2018
Building logical qubits in a superconducting quantum computing system Gambetta, Jay M.; Chow, Jerry M.; Steffen, Matthias npj Quantum Information, Vol. 3, Issue 1 https://doi.org/10.1038/s41534-016-0004-0	journal	January 2017
Atomic Layer Deposition: An Overview George, Steven M. Chemical Reviews, Vol. 110, Issue 1, p. 111-131 https://doi.org/10.1021/cr900056b	journal	January 2010
Modeling Mechanism and Growth Reactions for New Nanofabrication Processes by Atomic Layer Deposition Elliott, Simon D.; Dey, Gangotri; Maimaiti, Yasheng Advanced Materials, Vol. 28, Issue 27 https://doi.org/10.1002/adma.201504043	journal	December 2015
In Situ Studies on Reaction Mechanisms in Atomic Layer Deposition Knapas, Kjell; Ritala, Mikko Critical Reviews in Solid State and Materials Sciences, Vol. 38, Issue 3 https://doi.org/10.1080/10408436.2012.693460	journal	January 2013
Quantifying Geometric Strain at the PbS QD-TiO ₂ Anode Interface and Its Effect on Electronic Structures Trejo, Orlando; Roelofs, Katherine E.; Xu, Shicheng Nano Letters, Vol. 15, Issue 12 https://doi.org/10.1021/acs.nanolett.5b02373	journal	November 2015
Exploring the local electronic structure and geometric arrangement of ALD Zn(O,S) buffer layers using X-ray absorption spectroscopy Dadlani, Anup L.; Trejo, Orlando; Acharya, Shinjita Journal of Materials Chemistry C, Vol. 3, Issue 47 https://doi.org/10.1039/C5TC02912K	journal	January 2015
ALD Zn(O,S) Thin Films’ Interfacial Chemical and Structural Configuration Probed by XAS Dadlani, Anup L.; Acharya, Shinjita; Trejo, Orlando ACS Applied Materials & Interfaces, Vol. 8, Issue 23 https://doi.org/10.1021/acsami.6b04000	journal	May 2016
Sulfur: not a “silent” element any more Jalilehvand, Farideh Chem. Soc. Rev., Vol. 35, Issue 12 https://doi.org/10.1039/B417595F	journal	January 2006
Theoretical approaches to x-ray absorption fine structure Rehr, J. J.; Albers, R. C. Reviews of Modern Physics, Vol. 72, Issue 3 https://doi.org/10.1103/RevModPhys.72.621	journal	July 2000
Ab initio theory and calculations of X-ray spectra Rehr, John J.; Kas, Joshua J.; Prange, Micah P. Comptes Rendus Physique, Vol. 10, Issue 6 https://doi.org/10.1016/j.crhy.2008.08.004	journal	July 2009
Parameter-free calculations of X-ray spectra with FEFF9 Rehr, John J.; Kas, Joshua J.; Vila, Fernando D. Physical Chemistry Chemical Physics, Vol. 12, Issue 21 https://doi.org/10.1039/b926434e	journal	January 2010
High-throughput computational X-ray absorption spectroscopy Mathew, Kiran; Zheng, Chen; Winston, Donald Scientific Data, Vol. 5, Issue 1 https://doi.org/10.1038/sdata.2018.151	journal	July 2018
In situ synchrotron based x-ray techniques as monitoring tools for atomic layer deposition Devloo-Casier, Kilian; Ludwig, Karl F.; Detavernier, Christophe Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 32, Issue 1 https://doi.org/10.1116/1.4851716	journal	January 2014
In situ synchrotron x-ray characterization of ZnO atomic layer deposition Fong, D. D.; Eastman, J. A.; Kim, S. K. Applied Physics Letters, Vol. 97, Issue 19 https://doi.org/10.1063/1.3514254	journal	November 2010
Evolution of Crystal Structure During the Initial Stages of ZnO Atomic Layer Deposition Boichot, R.; Tian, L.; Richard, M. -I. Chemistry of Materials, Vol. 28, Issue 2 https://doi.org/10.1021/acs.chemmater.5b04223	journal	January 2016
Observing the Nucleation Phase of Atomic Layer Deposition In Situ Mack, James F.; Van Stockum, Philip B.; Yemane, Yonas T. Chemistry of Materials, Vol. 24, Issue 22 https://doi.org/10.1021/cm302398v	journal	October 2012
The Problem with Determining Atomic Structure at the Nanoscale Billinge, S. J. L.; Levin, I. Science, Vol. 316, Issue 5824 https://doi.org/10.1126/science.1135080	journal	April 2007
Supervised Machine-Learning-Based Determination of Three-Dimensional Structure of Metallic Nanoparticles Timoshenko, Janis; Lu, Deyu; Lin, Yuewei The Journal of Physical Chemistry Letters, Vol. 8, Issue 20 https://doi.org/10.1021/acs.jpclett.7b02364	journal	October 2017
Automated generation and ensemble-learned matching of X-ray absorption spectra Zheng, Chen; Mathew, Kiran; Chen, Chi npj Computational Materials, Vol. 4, Issue 1 https://doi.org/10.1038/s41524-018-0067-x	journal	March 2018
Classification of local chemical environments from x-ray absorption spectra using supervised machine learning Carbone, Matthew R.; Yoo, Shinjae; Topsakal, Mehmet Physical Review Materials, Vol. 3, Issue 3 https://doi.org/10.1103/PhysRevMaterials.3.033604	journal	March 2019
TiO ₂ –ZnS Cascade Electron Transport Layer for Efficient Formamidinium Tin Iodide Perovskite Solar Cells Ke, Weijun; Stoumpos, Constantinos C.; Logsdon, Jenna Leigh Journal of the American Chemical Society, Vol. 138, Issue 45 https://doi.org/10.1021/jacs.6b08790	journal	November 2016
Solar cells with PbS quantum dot sensitized TiO ₂ –multiwalled carbon nanotube composites, sulfide-titania gel and tin sulfide coated C-fabric Kokal, Ramesh K.; Deepa, Melepurath; Kalluri, Ankarao Physical Chemistry Chemical Physics, Vol. 19, Issue 38 https://doi.org/10.1039/C7CP05582J	journal	January 2017
Performance enhancement of mesoporous TiO2-based perovskite solar cells by ZnS ultrathin-interfacial modification layer Shaikh, Shoyebmohamad F.; Kwon, Hyeok-Chan; Yang, Wooseok Journal of Alloys and Compounds, Vol. 738 https://doi.org/10.1016/j.jallcom.2017.12.199	journal	March 2018
Atomic layer deposition of ZnS via in situ production of H2S Bakke, J. R.; King, J. S.; Jung, H. J. Thin Solid Films, Vol. 518, Issue 19 https://doi.org/10.1016/j.tsf.2010.03.074	journal	July 2010
Design of an atomic layer deposition reactor for hydrogen sulfide compatibility Dasgupta, Neil P.; Mack, James F.; Langston, Michael C. Review of Scientific Instruments, Vol. 81, Issue 4, Article No. 044102 https://doi.org/10.1063/1.3384349	journal	April 2010
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav Computational Materials Science, Vol. 68 https://doi.org/10.1016/j.commatsci.2012.10.028	journal	February 2013
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Machine learning for molecular and materials science Butler, Keith T.; Davies, Daniel W.; Cartwright, Hugh Nature, Vol. 559, Issue 7715 https://doi.org/10.1038/s41586-018-0337-2	journal	July 2018
Random Forests Breiman, Leo Machine Learning, Vol. 45, Issue 1, p. 5-32 https://doi.org/10.1023/A:1010933404324	journal	January 2001
Bias in random forest variable importance measures: Illustrations, sources and a solution Strobl, Carolin; Boulesteix, Anne-Laure; Zeileis, Achim BMC Bioinformatics, Vol. 8, Issue 1 https://doi.org/10.1186/1471-2105-8-25	journal	January 2007
Polarized X-ray absorption spectroscopy and XPS of TiS3: S K- and Ti L-edge XANES and S and Ti 2p XPS Fleet, M. E.; Harmer, S. L.; Liu, X. Surface Science, Vol. 584, Issue 2-3 https://doi.org/10.1016/j.susc.2005.03.048	journal	June 2005
In Situ S K-Edge X-ray Absorption Spectroscopy for Understanding and Developing SO _x Storage Catalysts Dathe, Hendrik; Jentys, Andreas; Lercher, Johannes A. The Journal of Physical Chemistry B, Vol. 109, Issue 46 https://doi.org/10.1021/jp054336c	journal	October 2005
Reaction of H ₂ S and S ₂ with Metal/Oxide Surfaces: Band-Gap Size and Chemical Reactivity Rodriguez, José A.; Chaturvedi, Sanjay; Kuhn, Mark The Journal of Physical Chemistry B, Vol. 102, Issue 28 https://doi.org/10.1021/jp9815208	journal	June 1998
Adsorption and interaction of H2S/SO2 on TiO2 Yanxin, Chen; Yi, Jiang; Wenzhao, Li Catalysis Today, Vol. 50, Issue 1 https://doi.org/10.1016/S0920-5861(98)00460-X	journal	April 1999
Density Functional Theory Study of the Adsorption and Reaction of H ₂ S on TiO ₂ Rutile (110) and Anatase (101) Surfaces Huang, Wen-Fei; Chen, Hsin-Tsung; Lin, M. C. The Journal of Physical Chemistry C, Vol. 113, Issue 47 https://doi.org/10.1021/jp906948a	journal	October 2009
Investigation of the H2S poisoning process for sensing composite material based on carbon nanotubes and metal oxides Duan, Yichen; Pirolli, Laurent; Teplyakov, Andrew V. Sensors and Actuators B: Chemical, Vol. 235 https://doi.org/10.1016/j.snb.2016.05.014	journal	November 2016
The complete reaction mechanism of H ₂ S desulfurization on an anatase TiO ₂ (001) surface: a density functional theory investigation Junkaew, Anchalee; Maitarad, Phornphimon; Arróyave, Raymundo Catalysis Science & Technology, Vol. 7, Issue 2 https://doi.org/10.1039/C6CY02030E	journal	January 2017
Steps on anatase TiO2(101) Gong, Xue-Qing; Selloni, Annabella; Batzill, Matthias Nature Materials, Vol. 5, Issue 8 https://doi.org/10.1038/nmat1695	journal	July 2006
Atomic Layer Deposition of Zinc Oxide: Diethyl Zinc Reactions and Surface Saturation from First-Principles Weckman, Timo; Laasonen, Kari The Journal of Physical Chemistry C, Vol. 120, Issue 38 https://doi.org/10.1021/acs.jpcc.6b06141	journal	September 2016

Similar Records

In situ x-ray studies of the incipient ZnO atomic layer deposition on

{In}_{0.53} {Ga}_{0.47} As

Journal Article · Mon Apr 27 00:00:00 EDT 2020 · Physical Review Materials · OSTI ID:1598269

Skopin, E. V.; Rapenne, L.; Deschanvres, J. L.; +6 more

Towards ALD thin film stabilized single-atom Pd ₁ catalysts

Journal Article · Wed Jul 27 00:00:00 EDT 2016 · Nanoscale · OSTI ID:1598269

Piernavieja-Hermida, Mar; Lu, Zheng; White, Anderson; +5 more

Ultrathin Amorphous Titania on Nanowires: Optimization of Conformal Growth and Elucidation of Atomic-Scale Motifs

Journal Article · Tue Apr 30 00:00:00 EDT 2019 · Nano Letters · OSTI ID:1598269

Yan, Danhua; Topsakal, Mehmet; Selcuk, Sencer; +11 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Elucidating the Evolving Atomic Structure in Atomic Layer Deposition Reactions with in Situ XANES and Machine Learning

Citation Formats

References (42)

Similar Records

Related Subjects