Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS3

Kevin M. Roccapriore; Nan Huang; Mark P. Oxley; Vinit Sharma; Timothy Taylor; Swagata Acharya; Dimitar Pashov; Mikhail I. Katsnelson; David Mandrus; Janice L. Musfeldt; Sergei V. Kalinin

doi:10.1021/acsnano.2c06253

Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS₃

Kevin M. Roccapriore^*, Nan Huang, Mark P. Oxley, Vinit Sharma, Timothy Taylor, Swagata Acharya, Dimitar Pashov, Mikhail I. Katsnelson, David Mandrus, Janice L. Musfeldt, Sergei V. Kalinin

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. We pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

Original language	English
Pages (from-to)	16713-16723
Number of pages	11
Journal	ACS Nano
Volume	16
Issue number	10
Early online date	29 Sept 2022
DOIs	https://doi.org/10.1021/acsnano.2c06253
Publication status	Published - 25 Oct 2022

Keywords

atomic defects
edge plasmon
electron irradiation
metal phosphorus trichalcogenides
moiré superlattice
scanning transmission electron microscopy
two-dimensional semiconductors

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10.1021/acsnano.2c06253

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@article{1092b3787f86494ebef32c92d90a4045,

title = "Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS3",

abstract = "Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moir{\'e} pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. We pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale. ",

keywords = "atomic defects, edge plasmon, electron irradiation, metal phosphorus trichalcogenides, moir{\'e} superlattice, scanning transmission electron microscopy, two-dimensional semiconductors",

author = "Roccapriore, {Kevin M.} and Nan Huang and Oxley, {Mark P.} and Vinit Sharma and Timothy Taylor and Swagata Acharya and Dimitar Pashov and Katsnelson, {Mikhail I.} and David Mandrus and Musfeldt, {Janice L.} and Kalinin, {Sergei V.}",

note = "Funding Information: This effort (electron microscopy) is based upon work supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division (K.M.R., S.V.K.) and was performed and partially supported at the Oak Ridge National Laboratory{\textquoteright}s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. This research used resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC05-00OR22725. V.S. acknowledges the XSEDE allocation (grant no. TG- DMR200008) and the Infrastructure for Scientific Applications and Advanced Computing (ISAAC) at the University of Tennessee for the computational resources. Research at the University of Tennessee is supported by the U.S. DOE, BES, Physical Behavior of Materials under award DE-SC00023144 (J.L.M.). N.H. and D.M. were supported by the National Science Foundation through grant number DMR-1808964. M.I.K. and S.A. are supported by the ERC Synergy Grant, project 854843 FASTCORR (ultrafast dynamics of correlated electrons in solids). D.P. is supported by the National Renewable Energy Laboratories. S.A., D.P., and M.I.K. acknowledge PRACE for awarding us access to Juwels Booster and Cluster, Germany. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = oct,

day = "25",

doi = "10.1021/acsnano.2c06253",

language = "English",

volume = "16",

pages = "16713--16723",

journal = "ACS Nano",

issn = "1936-0851",

publisher = "American Chemical Society",

number = "10",

}

TY - JOUR

T1 - Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS3

AU - Roccapriore, Kevin M.

AU - Huang, Nan

AU - Oxley, Mark P.

AU - Sharma, Vinit

AU - Taylor, Timothy

AU - Acharya, Swagata

AU - Pashov, Dimitar

AU - Katsnelson, Mikhail I.

AU - Mandrus, David

AU - Musfeldt, Janice L.

AU - Kalinin, Sergei V.

N1 - Funding Information: This effort (electron microscopy) is based upon work supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division (K.M.R., S.V.K.) and was performed and partially supported at the Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. This research used resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under contract no. DE-AC05-00OR22725. V.S. acknowledges the XSEDE allocation (grant no. TG- DMR200008) and the Infrastructure for Scientific Applications and Advanced Computing (ISAAC) at the University of Tennessee for the computational resources. Research at the University of Tennessee is supported by the U.S. DOE, BES, Physical Behavior of Materials under award DE-SC00023144 (J.L.M.). N.H. and D.M. were supported by the National Science Foundation through grant number DMR-1808964. M.I.K. and S.A. are supported by the ERC Synergy Grant, project 854843 FASTCORR (ultrafast dynamics of correlated electrons in solids). D.P. is supported by the National Renewable Energy Laboratories. S.A., D.P., and M.I.K. acknowledge PRACE for awarding us access to Juwels Booster and Cluster, Germany. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/10/25

Y1 - 2022/10/25

N2 - Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. We pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

AB - Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. We pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

KW - atomic defects

KW - edge plasmon

KW - electron irradiation

KW - metal phosphorus trichalcogenides

KW - moiré superlattice

KW - scanning transmission electron microscopy

KW - two-dimensional semiconductors

UR - http://www.scopus.com/inward/record.url?scp=85139398165&partnerID=8YFLogxK

U2 - 10.1021/acsnano.2c06253

DO - 10.1021/acsnano.2c06253

M3 - Article

AN - SCOPUS:85139398165

SN - 1936-0851

VL - 16

SP - 16713

EP - 16723

JO - ACS Nano

JF - ACS Nano

IS - 10

ER -

Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS₃

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