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.; Liang, Liangbo; Dyck, Ondrej; Berlijn, Tom; Eres, Gyula; Rouleau, Christopher M.; Xiao, Kai; Geohegan, David B.

doi:10.1021/acsnano.2c09952

Real-Time Diagnostics of 2D Crystal Transformations by Pulsed Laser Deposition: Controlled Synthesis of Janus WSSe Monolayers and Alloys

Journal Article · Tue Jan 17 00:00:00 EST 2023 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.2c09952· OSTI ID:1996711

^[1]; Lin, Yu-Chuan ^[2]; ^[1]; ^[1]; ^[1]; ^[1]; ^[3]; ^[1]; ^[1]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Pennsylvania State Univ., University Park, PA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division

Energetic processing methods such as hyperthermal implantation hold special promise to achieve the precision synthesis of metastable two-dimensional (2D) materials such as Janus monolayers; however, they require precise control. Here, we report a feedback approach to reveal and control the transformation pathways in materials synthesis by pulsed laser deposition (PLD) and apply it to investigate the transformation kinetics of monolayer WS₂ crystals into Janus WSSe and WSe₂ by implantation of Se clusters with different maximum kinetic energies (<42 eV/Se-atom) generated by laser ablation of a Se target. Real-time Raman spectroscopy and photoluminescence are used to assess the structure, composition, and optoelectronic quality of the monolayer crystal as it is implanted with well-controlled fluxes of selenium for different kinetic energies that are regulated with in situ ICCD imaging, ion probe, and spectroscopy diagnostics. First-principles calculations, XPS, and atomic-resolution HAADF STEM imaging are used to understand the intermediate alloy compositions and their vibrational modes to identify transformation pathways. The real-time kinetics measurements reveal highly selective top-layer conversion as WS₂ transforms through WS_2(1–x)Se_2x alloys to WSe₂ and provide the means to adjust processing conditions to achieve fractional and complete Janus WSSe monolayers as metastable transition states. The general approach demonstrates a real-time feedback method to achieve Janus layers or other metastable alloys of the desired composition, and a general means to adjust the structure and quality of materials grown by PLD, addressing priority research directions for precision synthesis with real-time adaptive control.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1996711

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 3 Vol. 17; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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2D materials
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Janus monolayers
alloys
implantation
in situ Raman
in situ photoluminescence
kinetics
layers
monolayers
pulsed laser deposition
transition-metal dichalcogenides

Real-Time Diagnostics of 2D Crystal Transformations by Pulsed Laser Deposition: Controlled Synthesis of Janus WSSe Monolayers and Alloys

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