Autonomous Synthesis of Thin Film Materials with Pulsed Laser Deposition Enabled by In Situ Spectroscopy and Automation

Harris, Sumner B.; Biswas, Arpan; Yun, Seok Joon; Roccapriore, Kevin M.; Rouleau, Christopher M.; Puretzky, Alexander A.; Vasudevan, Rama K.; Geohegan, David B.; Xiao, Kai

doi:10.1002/smtd.202301763

Title: Autonomous Synthesis of Thin Film Materials with Pulsed Laser Deposition Enabled by In Situ Spectroscopy and Automation

Journal Article · 28 April 2024 · Small Methods

DOI: https://doi.org/10.1002/smtd.202301763 · OSTI ID:2438990

^[1]; Biswas, Arpan ^[1];

^[1]; Roccapriore, Kevin M. ^[1];

^[1];

^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Autonomous systems that combine synthesis, characterization, and artificial intelligence can greatly accelerate the discovery and optimization of materials, however platforms for growth of macroscale thin films by physical vapor deposition techniques have lagged far behind others. Here this study demonstrates autonomous synthesis by pulsed laser deposition (PLD), a highly versatile synthesis technique, in the growth of ultrathin WSe₂ films. Further, by combing the automation of PLD synthesis and in situ diagnostic feedback with a high-throughput methodology, this study demonstrates a workflow and platform which uses Gaussian process regression and Bayesian optimization to autonomously identify growth regimes for WSe₂ films based on Raman spectral criteria by efficiently sampling 0.25% of the chosen 4D parameter space. With throughputs at least 10x faster than traditional PLD workflows, this platform and workflow enables the accelerated discovery and autonomous optimization of the vast number of materials that can be synthesized by PLD.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2438990

Journal Information:: Small Methods, Journal Name: Small Methods Vol. n/a; ISSN 2366-9608

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (55)

Artificial Chemist: An Autonomous Quantum Dot Synthesis Bot Epps, Robert W.; Bowen, Michael S.; Volk, Amanda A. Advanced Materials, Vol. 32, Issue 30 https://doi.org/10.1002/adma.202001626	journal	June 2020
Growth of Centimeter-Scale Monolayer and Few-Layer WSe ₂ Thin Films on SiO ₂ /Si Substrate via Pulsed Laser Deposition Seo, Sehun; Choi, Hojoong; Kim, So-Young Advanced Materials Interfaces, Vol. 5, Issue 20 https://doi.org/10.1002/admi.201800524	journal	June 2018
Direct In Situ Growth of Centimeter‐Scale Multi‐Heterojunction MoS ₂ /WS ₂ /WSe ₂ Thin‐Film Catalyst for Photo‐Electrochemical Hydrogen Evolution Seo, Sehun; Kim, Seungkyu; Choi, Hojoong Advanced Science, Vol. 6, Issue 13 https://doi.org/10.1002/advs.201900301	journal	April 2019
Scaling law for strain dependence of Raman spectra in transition‐metal dichalcogenides Zhang, Ye; Guo, Huaihong; Sun, Wei Journal of Raman Spectroscopy, Vol. 51, Issue 8 https://doi.org/10.1002/jrs.5908	journal	June 2020
Recent advances in autonomous synthesis of materials Li, Yucen; Xia, Lingling; Fan, Yiming ChemPhysMater, Vol. 1, Issue 2 https://doi.org/10.1016/j.chphma.2021.10.002	journal	April 2022
In-situ angle-resolved photoemission spectroscopy of copper-oxide thin films synthesized by molecular beam epitaxy Kim, Chung Koo; Drozdov, Ilya K.; Fujita, Kazuhiro Journal of Electron Spectroscopy and Related Phenomena https://doi.org/10.1016/j.elspec.2018.07.003	journal	September 2018
COMBO: An efficient Bayesian optimization library for materials science Ueno, Tsuyoshi; Rhone, Trevor David; Hou, Zhufeng Materials Discovery, Vol. 4 https://doi.org/10.1016/j.md.2016.04.001	journal	June 2016
NexusLIMS: A Laboratory Information Management System for Shared-Use Electron Microscopy Facilities Taillon, Joshua A.; Bina, Thomas F.; Plante, Raymond L. Microscopy and Microanalysis, Vol. 27, Issue 3 https://doi.org/10.1017/S1431927621000222	journal	April 2021
Tailoring Vacancies Far Beyond Intrinsic Levels Changes the Carrier Type and Optical Response in Monolayer MoSe _{2− x} Crystals Mahjouri-Samani, Masoud; Liang, Liangbo; Oyedele, Akinola Nano Letters, Vol. 16, Issue 8 https://doi.org/10.1021/acs.nanolett.6b02263	journal	July 2016
Nonequilibrium Synthesis of TiO ₂ Nanoparticle “Building Blocks” for Crystal Growth by Sequential Attachment in Pulsed Laser Deposition Mahjouri-Samani, Masoud; Tian, Mengkun; Puretzky, Alexander A. Nano Letters, Vol. 17, Issue 8 https://doi.org/10.1021/acs.nanolett.7b01047	journal	July 2017
Rapid Characterization and Parameter Space Exploration of Perovskites Using an Automated Routine Reinhardt, Elisabeth; Salaheldin, Ahmed M.; Distaso, Monica ACS Combinatorial Science, Vol. 22, Issue 1 https://doi.org/10.1021/acscombsci.9b00068	journal	December 2019
Real-Time Diagnostics of 2D Crystal Transformations by Pulsed Laser Deposition: Controlled Synthesis of Janus WSSe Monolayers and Alloys Harris, Sumner B.; Lin, Yu-Chuan; Puretzky, Alexander A. ACS Nano, Vol. 17, Issue 3 https://doi.org/10.1021/acsnano.2c09952	journal	January 2023
Large-Area Deposition of MoS 2 by Pulsed Laser Deposition with In Situ Thickness Control Serna, Martha I.; Yoo, Seong H.; Moreno, Salvador ACS Nano, Vol. 10, Issue 6 https://doi.org/10.1021/acsnano.6b01636	journal	May 2016
Low Energy Implantation into Transition-Metal Dichalcogenide Monolayers to Form Janus Structures Lin, Yu-Chuan; Liu, Chenze; Yu, Yiling ACS Nano, Vol. 14, Issue 4 https://doi.org/10.1021/acsnano.9b10196	journal	March 2020
Discovery of Wall-Selective Carbon Nanotube Growth Conditions via Automated Experimentation Nikolaev, Pavel; Hooper, Daylond; Perea-López, Nestor ACS Nano, Vol. 8, Issue 10 https://doi.org/10.1021/nn503347a	journal	October 2014
A Taxonomy of Global Optimization Methods Based on Response Surfaces Jones, Donald R. Journal of Global Optimization, Vol. 21, Issue 4, p. 345-383 https://doi.org/10.1023/A:1012771025575	journal	December 2001
Autonomy in materials research: a case study in carbon nanotube growth Nikolaev, Pavel; Hooper, Daylond; Webber, Frederick npj Computational Materials, Vol. 2, Issue 1 https://doi.org/10.1038/npjcompumats.2016.31	journal	October 2016
Impact of high-throughput screening in biomedical research Macarron, Ricardo; Banks, Martyn N.; Bojanic, Dejan Nature Reviews Drug Discovery, Vol. 10, Issue 3 https://doi.org/10.1038/nrd3368	journal	March 2011
AlphaFlow: autonomous discovery and optimization of multi-step chemistry using a self-driven fluidic lab guided by reinforcement learning Volk, Amanda A.; Epps, Robert W.; Yonemoto, Daniel T. Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-37139-y	journal	March 2023
Accelerating materials discovery using artificial intelligence, high performance computing and robotics Pyzer-Knapp, Edward O.; Pitera, Jed W.; Staar, Peter W. J. npj Computational Materials, Vol. 8, Issue 1 https://doi.org/10.1038/s41524-022-00765-z	journal	April 2022
A dynamic Bayesian optimized active recommender system for curiosity-driven partially Human-in-the-loop automated experiments Biswas, Arpan; Liu, Yongtao; Creange, Nicole npj Computational Materials, Vol. 10, Issue 1 https://doi.org/10.1038/s41524-023-01191-5	journal	February 2024
A mobile robotic chemist Burger, Benjamin; Maffettone, Phillip M.; Gusev, Vladimir V. Nature, Vol. 583, Issue 7815 https://doi.org/10.1038/s41586-020-2442-2	journal	July 2020
Bayesian reaction optimization as a tool for chemical synthesis Shields, Benjamin J.; Stevens, Jason; Li, Jun Nature, Vol. 590, Issue 7844 https://doi.org/10.1038/s41586-021-03213-y	journal	February 2021
SciPy 1.0: fundamental algorithms for scientific computing in Python Virtanen, Pauli; Gommers, Ralf; Oliphant, Travis E. Nature Methods https://doi.org/10.1038/s41592-019-0686-2	journal	February 2020
Efficient Closed-loop Maximization of Carbon Nanotube Growth Rate using Bayesian Optimization Chang, Jorge; Nikolaev, Pavel; Carpena-Núñez, Jennifer Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-64397-3	journal	June 2020
Autonomous materials discovery driven by Gaussian process regression with inhomogeneous measurement noise and anisotropic kernels Noack, Marcus M.; Doerk, Gregory S.; Li, Ruipeng Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-74394-1	journal	October 2020
The rise of self-driving labs in chemical and materials sciences Abolhasani, Milad; Kumacheva, Eugenia Nature Synthesis, Vol. 2, Issue 6 https://doi.org/10.1038/s44160-022-00231-0	journal	January 2023
Origin and evolution of high throughput screening Pereira, D. A.; Williams, J. A. British Journal of Pharmacology, Vol. 152, Issue 1 https://doi.org/10.1038/sj.bjp.0707373	journal	September 2007
Focused helium-ion beam irradiation effects on electrical transport properties of few-layer WSe2: enabling nanoscale direct write homo-junctions Stanford, Michael G.; Pudasaini, Pushpa Raj; Belianinov, Alex Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep27276	journal	June 2016
Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material Zhang, Xin; Qiao, Xiao-Fen; Shi, Wei Chemical Society Reviews, Vol. 44, Issue 9 https://doi.org/10.1039/C4CS00282B	journal	January 2015
Automated microfluidic platform for systematic studies of colloidal perovskite nanocrystals: towards continuous nano-manufacturing Epps, Robert W.; Felton, Kobi C.; Coley, Connor W. Lab on a Chip, Vol. 17, Issue 23 https://doi.org/10.1039/C7LC00884H	journal	January 2017
Quantifying local thickness and composition in thin films of organic photovoltaic blends by Raman scattering Rodríguez-Martínez, Xabier; Vezie, Michelle S.; Shi, Xingyuan Journal of Materials Chemistry C, Vol. 5, Issue 29 https://doi.org/10.1039/C7TC01472D	journal	January 2017
Constrained Bayesian optimization for automatic chemical design using variational autoencoders Griffiths, Ryan-Rhys; Hernández-Lobato, José Miguel Chemical Science, Vol. 11, Issue 2 https://doi.org/10.1039/C9SC04026A	journal	January 2020
Toward autonomous design and synthesis of novel inorganic materials Szymanski, Nathan J.; Zeng, Yan; Huo, Haoyan Materials Horizons, Vol. 8, Issue 8 https://doi.org/10.1039/D1MH00495F	journal	January 2021
Optical functions of silicon at elevated temperatures Jellison, G. E.; Modine, F. A. Journal of Applied Physics, Vol. 76, Issue 6 https://doi.org/10.1063/1.357378	journal	September 1994
Highly crystalline MoS ₂ thin films grown by pulsed laser deposition Serrao, Claudy R.; Diamond, Anthony M.; Hsu, Shang-Lin Applied Physics Letters, Vol. 106, Issue 5 https://doi.org/10.1063/1.4907169	journal	February 2015
Guided search for desired functional responses via Bayesian optimization of generative model: Hysteresis loop shape engineering in ferroelectrics Kalinin, Sergei V.; Ziatdinov, Maxim; Vasudevan, Rama K. Journal of Applied Physics, Vol. 128, Issue 2 https://doi.org/10.1063/5.0011917	journal	July 2020
Autonomous materials synthesis by machine learning and robotics Shimizu, Ryota; Kobayashi, Shigeru; Watanabe, Yuki APL Materials, Vol. 8, Issue 11 https://doi.org/10.1063/5.0020370	journal	November 2020
Multi-objective Bayesian optimization of ferroelectric materials with interfacial control for memory and energy storage applications Biswas, Arpan; Morozovska, Anna N.; Ziatdinov, Maxim Journal of Applied Physics, Vol. 130, Issue 20 https://doi.org/10.1063/5.0068903	journal	November 2021
In situ laser reflectivity to monitor and control the nucleation and growth of atomically thin 2D materials* Puretzky, Alexander A.; Lin, Yu-Chuan; Liu, Chenze 2D Materials, Vol. 7, Issue 2 https://doi.org/10.1088/2053-1583/ab7a72	journal	March 2020
Optimizing training trajectories in variational autoencoders via latent Bayesian optimization approach ^* Biswas, Arpan; Vasudevan, Rama; Ziatdinov, Maxim Machine Learning: Science and Technology, Vol. 4, Issue 1 https://doi.org/10.1088/2632-2153/acb316	journal	February 2023
Taking the Human Out of the Loop: A Review of Bayesian Optimization Shahriari, Bobak; Swersky, Kevin; Wang, Ziyu Proceedings of the IEEE, Vol. 104, Issue 1 https://doi.org/10.1109/JPROC.2015.2494218	journal	January 2016
A New Method of Locating the Maximum Point of an Arbitrary Multipeak Curve in the Presence of Noise Kushner, H. J. Journal of Basic Engineering, Vol. 86, Issue 1 https://doi.org/10.1115/1.3653121	journal	March 1964
An Approach to Bayesian Optimization for Design Feasibility Check on Discontinuous Black-Box Functions Biswas, Arpan; Hoyle, Christopher Journal of Mechanical Design, Vol. 143, Issue 3 https://doi.org/10.1115/1.4049742	journal	February 2021
A Bayesian experimental autonomous researcher for mechanical design Gongora, Aldair E.; Xu, Bowen; Perry, Wyatt Science Advances, Vol. 6, Issue 15 https://doi.org/10.1126/sciadv.aaz1708	journal	April 2020
Self-driving laboratory for accelerated discovery of thin-film materials MacLeod, B. P.; Parlane, F. G. L.; Morrissey, T. D. Science Advances, Vol. 6, Issue 20 https://doi.org/10.1126/sciadv.aaz8867	journal	May 2020
Synthesis of Novel Thin-Film Materials by Pulsed Laser Deposition Lowndes, D. H.; Geohegan, D. B.; Puretzky, A. A. Science, Vol. 273, Issue 5277, p. 898-903 https://doi.org/10.1126/science.273.5277.898	journal	August 1996
Quick Optical Identification of the Defect Formation in Monolayer WSe2 for Growth Optimization Fang, Long; Chen, Haitao; Yuan, Xiaoming Nanoscale Research Letters, Vol. 14, Issue 1 https://doi.org/10.1186/s11671-019-3110-z	journal	August 2019
Machine-learning-assisted analysis of transition metal dichalcogenide thin-film growth Kim, Hyuk Jin; Chong, Minsu; Rhee, Tae Gyu Nano Convergence, Vol. 10, Issue 1 https://doi.org/10.1186/s40580-023-00359-5	journal	February 2023
Bayesian auxiliary variable models for binary and multinomial regression Held, Leonhard; Holmes, Chris C. Bayesian Analysis, Vol. 1, Issue 1 https://doi.org/10.1214/06-BA105	journal	March 2006
Measuring the optical permittivity of two-dimensional materials without a priori knowledge of electronic transitions Jung, Gwang-Hun; Yoo, SeokJae; Park, Q-Han Nanophotonics, Vol. 8, Issue 2 https://doi.org/10.1515/nanoph-2018-0120	journal	September 2018
Bayesian Optimization in a Billion Dimensions via Random Embeddings Wang, Ziyu; Hutter, Frank; Zoghi, Masrour Journal of Artificial Intelligence Research, Vol. 55 https://doi.org/10.1613/jair.4806	journal	January 2016
Basic Research Needs Workshop on Synthesis Science for Energy Relevant Technology De Yoreo, Jim; Mandrus, David; Soderholm, Lynda https://doi.org/10.2172/1616513	report	May 2016
Quick Optical Identification of the Defect Formation in Monolayer WSe2 for Growth Optimization Fang, Long; Chen, Haitao; Yuan, Xiaoming figshare https://doi.org/10.6084/m9.figshare.c.4618286	collection	January 2019
Machine-learning-assisted analysis of transition metal dichalcogenide thin-film growth Kim, Hyuk Jin; Chong, Minsu; Rhee, Tae Gyu figshare https://doi.org/10.6084/m9.figshare.c.6576628	collection	January 2023

Similar Records

Towards Automated Design of Corrosion Resistant Alloy Coatings with an Autonomous Scanning Droplet Cell

Journal Article · 2022 · JOM. Journal of the Minerals, Metals & Materials Society · OSTI ID:1878621

DeCost, Brian; Joress, Howie; Sarker, Suchismita; +2 more

Deep learning with plasma plume image sequences for anomaly detection and prediction of growth kinetics during pulsed laser deposition

Journal Article · 2024 · npj Computational Materials · OSTI ID:2350729

Harris, Sumner B.; Rouleau, Christopher M.; Xiao, Kai; +1 more

Online Bayesian State Estimation for Real-Time Monitoring of Growth Kinetics in Thin Film Synthesis

Journal Article · 2025 · Nano Letters · OSTI ID:2538227

Harris, Sumner B.; López Fajardo, Ruth Y.; Puretzky, Alexander A.; +3 more

Related Subjects

36 MATERIALS SCIENCE
automation
autonomous synthesis
in situ diagnostics
machine learning
pulsed laser deposition

Title: Autonomous Synthesis of Thin Film Materials with Pulsed Laser Deposition Enabled by In Situ Spectroscopy and Automation

Citation Formats

References (55)

Similar Records

Related Subjects