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 -