Autonomous scanning probe microscopy investigations over WS2 and Au{111}

Thomas, John C.; Rossi, Antonio; Smalley, Darian; Francaviglia, Luca; Yu, Zhuohang; Zhang, Tianyi; Kumari, Shalini; Robinson, Joshua A.; Terrones, Mauricio; Ishigami, Masahiro; Rotenberg, Eli; Barnard, Edward S.; Raja, Archana; Wong, Ed; Ogletree, D. Frank; Noack, Marcus M.; Weber-Bargioni, Alexander

doi:10.1038/s41524-022-00777-9

Title: Autonomous scanning probe microscopy investigations over WS2 and Au{111}

Journal Article · Sun May 01 20:00:00 EDT 2022 · npj Computational Materials

DOI: https://doi.org/10.1038/s41524-022-00777-9 · OSTI ID:1865998

; Rossi, Antonio; Smalley, Darian;

; Yu, Zhuohang; Zhang, Tianyi; Kumari, Shalini; Robinson, Joshua A.; Terrones, Mauricio; Ishigami, Masahiro; Rotenberg, Eli;

; Raja, Archana; Wong, Ed;

;

; Weber-Bargioni, Alexander

Abstract Individual atomic defects in 2D materials impact their macroscopic functionality. Correlating the interplay is challenging, however, intelligent hyperspectral scanning tunneling spectroscopy (STS) mapping provides a feasible solution to this technically difficult and time consuming problem. Here, dense spectroscopic volume is collected autonomously via Gaussian process regression, where convolutional neural networks are used in tandem for spectral identification. Acquired data enable defect segmentation, and a workflow is provided for machine-driven decision making during experimentation with capability for user customization. We provide a means towards autonomous experimentation for the benefit of both enhanced reproducibility and user-accessibility. Hyperspectral investigations on WS ₂ sulfur vacancy sites are explored, which is combined with local density of states confirmation on the Au{111} herringbone reconstruction. Chalcogen vacancies, pristine WS ₂ , Au face-centered cubic, and Au hexagonal close-packed regions are examined and detected by machine learning methods to demonstrate the potential of artificial intelligence for hyperspectral STS mapping.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); Swiss National Science Foundation (SNSF); USDOE; USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1865998

Journal Information:: npj Computational Materials, Journal Name: npj Computational Materials Journal Issue: 1 Vol. 8; ISSN 2057-3960

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (67)

Recent Progress on the Scanning Tunneling Microscopy and Spectroscopy Study of Semiconductor Heterojunctions Peng, Wenbing; Wang, Haolin; Lu, Hui Small, Vol. 17, Issue 50 https://doi.org/10.1002/smll.202100655	journal	August 2021
The future of gold in electronics Ellis, Timothy W. Gold Bulletin, Vol. 37, Issue 1-2 https://doi.org/10.1007/BF03215518	journal	March 2004
Current imaging tunneling spectroscopy of metallic deposits on silicon Asenjo, A.; Gómez-Rodríguez, J. M.; Baró, A. M. Ultramicroscopy, Vol. 42-44 https://doi.org/10.1016/0304-3991(92)90381-S	journal	July 1992
Automated tip functionalization via machine learning in scanning probe microscopy Alldritt, Benjamin; Urtev, Fedor; Oinonen, Niko Computer Physics Communications, Vol. 273 https://doi.org/10.1016/j.cpc.2021.108258	journal	April 2022
Comparative study of hyperspectral image classification by multidimensional Convolutional Neural Network approaches to improve accuracy Ortac, Gizem; Ozcan, Giyasettin Expert Systems with Applications, Vol. 182 https://doi.org/10.1016/j.eswa.2021.115280	journal	November 2021
Correcting nonlinear drift distortion of scanning probe and scanning transmission electron microscopies from image pairs with orthogonal scan directions Ophus, Colin; Ciston, Jim; Nelson, Chris T. Ultramicroscopy, Vol. 162 https://doi.org/10.1016/j.ultramic.2015.12.002	journal	March 2016
Four-Dimensional Scanning Transmission Electron Microscopy (4D-STEM): From Scanning Nanodiffraction to Ptychography and Beyond Ophus, Colin Microscopy and Microanalysis, Vol. 25, Issue 3 https://doi.org/10.1017/S1431927619000497	journal	May 2019
Atomistic Positioning of Defects in Helium Ion Treated Single-Layer MoS ₂ Mitterreiter, Elmar; Schuler, Bruno; Cochrane, Katherine A. Nano Letters, Vol. 20, Issue 6 https://doi.org/10.1021/acs.nanolett.0c01222	journal	May 2020
Machine Learning in Nanoscience: Big Data at Small Scales Brown, Keith A.; Brittman, Sarah; Maccaferri, Nicolò Nano Letters, Vol. 20, Issue 1 https://doi.org/10.1021/acs.nanolett.9b04090	journal	December 2019
Autonomous Experiments in Scanning Probe Microscopy and Spectroscopy: Choosing Where to Explore Polarization Dynamics in Ferroelectrics Vasudevan, Rama K.; Kelley, Kyle P.; Hinkle, Jacob ACS Nano, Vol. 15, Issue 7 https://doi.org/10.1021/acsnano.0c10239	journal	July 2021
Automated and Autonomous Experiments in Electron and Scanning Probe Microscopy Kalinin, Sergei V.; Ziatdinov, Maxim; Hinkle, Jacob ACS Nano, Vol. 15, Issue 8 https://doi.org/10.1021/acsnano.1c02104	journal	July 2021
Revealing the Chemical Bonding in Adatom Arrays via Machine Learning of Hyperspectral Scanning Tunneling Spectroscopy Data Roccapriore, Kevin M.; Zou, Qiang; Zhang, Lizhi ACS Nano, Vol. 15, Issue 7 https://doi.org/10.1021/acsnano.1c02902	journal	June 2021
Defect-Tolerant Aligned Dipoles within Two-Dimensional Plastic Lattices Thomas, John C.; Schwartz, Jeffrey J.; Hohman, J. Nathan ACS Nano, Vol. 9, Issue 5 https://doi.org/10.1021/acsnano.5b01329	journal	April 2015
Autonomous Scanning Probe Microscopy in Situ Tip Conditioning through Machine Learning Rashidi, Mohammad; Wolkow, Robert A. ACS Nano, Vol. 12, Issue 6 https://doi.org/10.1021/acsnano.8b02208	journal	May 2018
How Substitutional Point Defects in Two-Dimensional WS ₂ Induce Charge Localization, Spin–Orbit Splitting, and Strain Schuler, Bruno; Lee, Jun-Ho; Kastl, Christoph ACS Nano, Vol. 13, Issue 9 https://doi.org/10.1021/acsnano.9b04611	journal	August 2019
Terahertz-Field-Driven Scanning Tunneling Luminescence Spectroscopy Kimura, Kensuke; Morinaga, Yuta; Imada, Hiroshi ACS Photonics, Vol. 8, Issue 4 https://doi.org/10.1021/acsphotonics.0c01755	journal	January 2021
Comparison of the structures and wetting properties of self-assembled monolayers of n-alkanethiols on the coinage metal surfaces, copper, silver, and gold Laibinis, Paul E.; Whitesides, George M.; Allara, David L. Journal of the American Chemical Society, Vol. 113, Issue 19 https://doi.org/10.1021/ja00019a011	journal	September 1991
Characterization of Self-Assembled Monolayers of Fullerene Derivatives on Gold Surfaces: Implications for Device Evaluations Shirai, Yasuhiro; Cheng, Long; Chen, Bo Journal of the American Chemical Society, Vol. 128, Issue 41 https://doi.org/10.1021/ja063451d	journal	September 2006
Analyzing the Motion of Benzene on Au{111}: Single Molecule Statistics from Scanning Probe Images Mantooth, Brent A.; Sykes, E. Charles H.; Han, Patrick The Journal of Physical Chemistry C, Vol. 111, Issue 17 https://doi.org/10.1021/jp0663558	journal	May 2007
Hyperspectral Nanoscale Imaging on Dielectric Substrates with Coaxial Optical Antenna Scan Probes. Weber-Bargioni, Alexander; Schwartzberg, Adam; Cornaglia, Matteo Nano Letters, Vol. 11, Issue 3 https://doi.org/10.1021/nl104163m	journal	March 2011
Valleytronics in 2D materials Schaibley, John R.; Yu, Hongyi; Clark, Genevieve Nature Reviews Materials, Vol. 1, Issue 11 https://doi.org/10.1038/natrevmats.2016.55	journal	August 2016
2D transition metal dichalcogenides Manzeli, Sajedeh; Ovchinnikov, Dmitry; Pasquier, Diego Nature Reviews Materials, Vol. 2, Issue 8 https://doi.org/10.1038/natrevmats.2017.33	journal	June 2017
Evolution of interlayer coupling in twisted molybdenum disulfide bilayers Liu, Kaihui; Zhang, Liming; Cao, Ting Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5966	journal	September 2014
Optically active quantum dots in monolayer WSe2 Srivastava, Ajit; Sidler, Meinrad; Allain, Adrien V. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.60	journal	May 2015
Cubes and slices Bannon, David Nature Photonics, Vol. 3, Issue 11 https://doi.org/10.1038/nphoton.2009.205	journal	November 2009
Ultrafast terahertz control of extreme tunnel currents through single atoms on a silicon surface Jelic, Vedran; Iwaszczuk, Krzysztof; Nguyen, Peter H. Nature Physics, Vol. 13, Issue 6 https://doi.org/10.1038/nphys4047	journal	February 2017
Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides Barja, Sara; Refaely-Abramson, Sivan; Schuler, Bruno Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11342-2	journal	July 2019
The role of chalcogen vacancies for atomic defect emission in MoS2 Mitterreiter, Elmar; Schuler, Bruno; Micevic, Ana Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-24102-y	journal	June 2021
Spin-dependent vibronic response of a carbon radical ion in two-dimensional WS2 Cochrane, Katherine A.; Lee, Jun-Ho; Kastl, Christoph Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-27585-x	journal	December 2021
Room-temperature optically detected magnetic resonance of single defects in hexagonal boron nitride Stern, Hannah L.; Gu, Qiushi; Jarman, John Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-28169-z	journal	February 2022
Deep neural networks for understanding noisy data applied to physical property extraction in scanning probe microscopy Borodinov, Nikolay; Neumayer, Sabine; Kalinin, Sergei V. npj Computational Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41524-019-0148-5	journal	February 2019
Machine-learned multi-system surrogate models for materials prediction Nyshadham, Chandramouli; Rupp, Matthias; Bekker, Brayden npj Computational Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41524-019-0189-9	journal	April 2019
Machine learning enabled autonomous microstructural characterization in 3D samples Chan, Henry; Cherukara, Mathew; Loeffler, Troy D. npj Computational Materials, Vol. 6, Issue 1 https://doi.org/10.1038/s41524-019-0267-z	journal	January 2020
Off-the-shelf deep learning is not enough, and requires parsimony, Bayesianity, and causality Vasudevan, Rama K.; Ziatdinov, Maxim; Vlcek, Lukas npj Computational Materials, Vol. 7, Issue 1 https://doi.org/10.1038/s41524-020-00487-0	journal	January 2021
Electron spin resonance of single iron phthalocyanine molecules and role of their non-localized spins in magnetic interactions Zhang, Xue; Wolf, Christoph; Wang, Yu Nature Chemistry, Vol. 14, Issue 1 https://doi.org/10.1038/s41557-021-00827-7	journal	November 2021
Correlated electronic phases in twisted bilayer transition metal dichalcogenides Wang, Lei; Shih, En-Min; Ghiotto, Augusto Nature Materials, Vol. 19, Issue 8 https://doi.org/10.1038/s41563-020-0708-6	journal	June 2020
Strongly correlated electrons and hybrid excitons in a moiré heterostructure Shimazaki, Yuya; Schwartz, Ido; Watanabe, Kenji Nature, Vol. 580, Issue 7804 https://doi.org/10.1038/s41586-020-2191-2	journal	April 2020
Computer vision distortion correction of scanning probe microscopy images Gaponenko, Iaroslav; Tückmantel, Philippe; Ziegler, Benedikt Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-00765-w	journal	April 2017
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
Artificial-intelligence-driven scanning probe microscopy Krull, A.; Hirsch, P.; Rother, C. Communications Physics, Vol. 3, Issue 1 https://doi.org/10.1038/s42005-020-0317-3	journal	March 2020
Gaussian processes for autonomous data acquisition at large-scale synchrotron and neutron facilities Noack, Marcus M.; Zwart, Petrus H.; Ushizima, Daniela M. Nature Reviews Physics, Vol. 3, Issue 10 https://doi.org/10.1038/s42254-021-00345-y	journal	July 2021
From the bottom up: dimensional control and characterization in molecular monolayers Claridge, Shelley A.; Liao, Wei-Ssu; Thomas, John C. Chem. Soc. Rev., Vol. 42, Issue 7 https://doi.org/10.1039/C2CS35365B	journal	January 2013
Engineering graphene and TMDs based van der Waals heterostructures for photovoltaic and photoelectrochemical solar energy conversion Li, Changli; Cao, Qi; Wang, Faze Chemical Society Reviews, Vol. 47, Issue 13 https://doi.org/10.1039/C8CS00067K	journal	January 2018
Atomic structure of defects and dopants in 2D layered transition metal dichalcogenides Wang, Shanshan; Robertson, Alex; Warner, Jamie H. Chemical Society Reviews, Vol. 47, Issue 17 https://doi.org/10.1039/C8CS00236C	journal	January 2018
Enabling autonomous scanning probe microscopy imaging of single molecules with deep learning Sotres, Javier; Boyd, Hannah; Gonzalez-Martinez, Juan F. Nanoscale, Vol. 13, Issue 20 https://doi.org/10.1039/D1NR01109J	journal	January 2021
Quantum emitters in 2D materials: Emitter engineering, photophysics, and integration in photonic nanostructures Kianinia, Mehran; Xu, Zai-Quan; Toth, Milos Applied Physics Reviews, Vol. 9, Issue 1 https://doi.org/10.1063/5.0072091	journal	March 2022
A review of hyperspectral imaging for nanoscale materials research Dong, Xingchen; Jakobi, Martin; Wang, Shengjia Applied Spectroscopy Reviews, Vol. 54, Issue 4 https://doi.org/10.1080/05704928.2018.1463235	journal	April 2018
Defect engineering of two-dimensional transition metal dichalcogenides Lin, Zhong; Carvalho, Bruno R.; Kahn, Ethan 2D Materials, Vol. 3, Issue 2 https://doi.org/10.1088/2053-1583/3/2/022002	journal	April 2016
Deep learning-guided surface characterization for autonomous hydrogen lithography Rashidi, Mohammad; Croshaw, Jeremiah; Mastel, Kieran Machine Learning: Science and Technology, Vol. 1, Issue 2 https://doi.org/10.1088/2632-2153/ab6d5e	journal	March 2020
Machine learning at the (sub)atomic scale: next generation scanning probe microscopy Gordon, Oliver M.; Moriarty, Philip J. Machine Learning: Science and Technology, Vol. 1, Issue 2 https://doi.org/10.1088/2632-2153/ab7d2f	journal	May 2020
K-means-driven Gaussian Process data collection for angle-resolved photoemission spectroscopy Melton, Charles N.; Noack, Marcus M.; Ohta, Taisuke Machine Learning: Science and Technology, Vol. 1, Issue 4 https://doi.org/10.1088/2632-2153/abab61	journal	October 2020
Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS 2 Schuler, Bruno; Qiu, Diana Y.; Refaely-Abramson, Sivan Physical Review Letters, Vol. 123, Issue 7 https://doi.org/10.1103/PhysRevLett.123.076801	journal	August 2019
Direct Measurement of Surface Diffusion Using Atom-Tracking Scanning Tunneling Microscopy Swartzentruber, B. S. Physical Review Letters, Vol. 76, Issue 3 https://doi.org/10.1103/PhysRevLett.76.459	journal	January 1996
Scanning Tunneling Microscopy Observation of an Electronic Superlattice at the Surface of Clean Gold Chen, W.; Madhavan, V.; Jamneala, T. Physical Review Letters, Vol. 80, Issue 7 https://doi.org/10.1103/PhysRevLett.80.1469	journal	February 1998
One dimensional convolutional neural networks and local binary patterns for hyperspectral image classification Miclea, Andreia Valentina; Terebes, Romulus; Meza, Serban 2020 IEEE International Conference on Automation, Quality and Testing, Robotics (AQTR) https://doi.org/10.1109/AQTR49680.2020.9129920	conference	May 2020
Displacement Measurement and Its Application in Interframe Image Coding Jain, J.; Jain, A. IEEE Transactions on Communications, Vol. 29, Issue 12 https://doi.org/10.1109/TCOM.1981.1094950	journal	December 1981
Vertical and lateral drift corrections of scanning probe microscopy images Rahe, P.; Bechstein, R.; Kühnle, A. Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 28, Issue 3 https://doi.org/10.1116/1.3360909	journal	May 2010
Electrically driven photon emission from individual atomic defects in monolayer WS ₂ Schuler, Bruno; Cochrane, Katherine A.; Kastl, Christoph Science Advances, Vol. 6, Issue 38 https://doi.org/10.1126/sciadv.abb5988	journal	September 2020
Autonomous robotic nanofabrication with reinforcement learning Leinen, Philipp; Esders, Malte; Schütt, Kristof T. Science Advances, Vol. 6, Issue 36 https://doi.org/10.1126/sciadv.abb6987	journal	September 2020
Single-Molecule Vibrational Spectroscopy and Microscopy Stipe, B. C. Science, Vol. 280, Issue 5370 https://doi.org/10.1126/science.280.5370.1732	journal	June 1998
Attosecond coherent manipulation of electrons in tunneling microscopy Garg, M.; Kern, K. Science, Vol. 367, Issue 6476 https://doi.org/10.1126/science.aaz1098	journal	November 2019
Scanning Tunneling Spectroscopy Zandvliet, Harold J. W.; van Houselt, Arie Annual Review of Analytical Chemistry, Vol. 2, Issue 1 https://doi.org/10.1146/annurev-anchem-060908-155213	journal	July 2009
Machine Learning in Materials Discovery: Confirmed Predictions and Their Underlying Approaches Saal, James E.; Oliynyk, Anton O.; Meredig, Bryce Annual Review of Materials Research, Vol. 50, Issue 1 https://doi.org/10.1146/annurev-matsci-090319-010954	journal	July 2020
Electronic Transport in Two-Dimensional Materials Sangwan, Vinod K.; Hersam, Mark C. Annual Review of Physical Chemistry, Vol. 69, Issue 1 https://doi.org/10.1146/annurev-physchem-050317-021353	journal	April 2018
Atomic-Resolution Surface Spectroscopy with the Scanning Tunneling Microscope Hamers, R. J. Annual Review of Physical Chemistry, Vol. 40, Issue 1 https://doi.org/10.1146/annurev.pc.40.100189.002531	journal	October 1989
The role of convolutional neural networks in scanning probe microscopy: a review Azuri, Ido; Rosenhek-Goldian, Irit; Regev-Rudzki, Neta Beilstein Journal of Nanotechnology, Vol. 12 https://doi.org/10.3762/bjnano.12.66	journal	January 2021
Gaussian Processes for Machine Learning Rasmussen, Carl Edward; Williams, Christopher K. I. The MIT Press https://doi.org/10.7551/mitpress/3206.001.0001	book	January 2005

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