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Thickness and Stacking Sequence Determination of Exfoliated Dichalcogenides (1T-TaS2, 2H-MoS2) Using Scanning Transmission Electron Microscopy

Published online by Cambridge University Press:  03 September 2018

Robert Hovden*
Affiliation:
School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA Department of Materials Science & Engineering, University of Michigan, Ann Arbor, MI48109, USA
Pengzi Liu
Affiliation:
School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA
Noah Schnitzer
Affiliation:
Department of Materials Science & Engineering, University of Michigan, Ann Arbor, MI48109, USA
Adam W. Tsen
Affiliation:
Department of Chemistry, University of Waterloo, Waterloo, ON, Canada, N2L 3G1
Yu Liu
Affiliation:
Key Laboratory of Materials Physics, Chinese Academy of Sciences, Hefei 230031, China
Wenjian Lu
Affiliation:
Key Laboratory of Materials Physics, Chinese Academy of Sciences, Hefei 230031, China
Yuping Sun
Affiliation:
Key Laboratory of Materials Physics, Chinese Academy of Sciences, Hefei 230031, China High Magnetic Field Laboratory, Chinese Academy of Sciences, Hefei 230031, China Centre of Advanced Microstructures, Nanjing University, Nanjing, 210093, China
Lena F. Kourkoutis
Affiliation:
School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA Kavli Institute at Cornell for Nanoscale Science, Ithaca, NY 14853, USA
*
*Authors for correspondence: Robert Hovden, E-mail: [email protected]; Lena Kourkoutis, [email protected]
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Abstract

Layered transition metal dichalcogenides (TMDs) have attracted interest due to their promise for future electronic and optoelectronic technologies. As one approaches the two-dimensional (2D) limit, thickness and local topology can greatly influence the macroscopic properties of a material. To understand the unique behavior of TMDs it is therefore important to identify the number of atomic layers and their stacking in a sample. The goal of this work is to extract the thickness and stacking sequence of TMDs directly by matching experimentally recorded high-angle annular dark-field scanning transmission electron microscope images and convergent-beam electron diffraction (CBED) patterns to quantum mechanical, multislice scattering simulations. Advantageously, CBED approaches do not require a resolved lattice in real space and are capable of neglecting the thickness contribution of amorphous surface layers. Here we demonstrate the crystal thickness can be determined from CBED in exfoliated 1T-TaS2 and 2H-MoS2 to within a single layer for ultrathin ≲9 layers and ±1 atomic layer (or better) in thicker specimens while also revealing information about stacking order—even when the crystal structure is unresolved in real space.

Type
Materials Science Applications
Copyright
© Microscopy Society of America 2018 

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References

Alden, JS, Tsen, AW, Huang, PY, Hovden, R, Brown, L, Park, J, Muller, DA McEuen, PL (2013) Strain solitons and topological defects in bilayer graphene. Proc Natl Acad Sci U S A 110, 1125611260.Google Scholar
Anstis, GR, Cai, DQ Cockayne, DJH (2003) Limitations on the s-state approach to the interpretation of sub-angstrom resolution electron microscope images and microanalysis. Ultramicroscopy 94, 309327.Google Scholar
Batson, PE, Dellby, N Krivanek, OL (2002) Sub-angstrom resolution using aberration corrected electron optics. Nature 418, 617620.Google Scholar
Bhattacharyya, S Singh, AK (2012) Semiconductor-metal transition in semiconducting bilayer sheets of transition-metal dichalcogenides. Phys Rev B 86, 075454.Google Scholar
Brown, L, Hovden, R, Huang, P, Wojcik, M, Muller, DA Park, J (2012) Twinning and twisting of tri- and bilayer graphene. Nano Letters 12, 16091615.Google Scholar
Crewe, A, Wall, J, Wall, J, Langmore, J Langmore, J (1970) Visibility of single atoms. Science 168, 13381340.Google Scholar
Dean, C, Young, AF, Wang, L, Meric, I, Lee, GH, Watanabe, K, Taniguchi, T, Shepard, K, Kim, P Hone, J (2012) Graphene based heterostructures. Solid State Commun 152, 12751282.Google Scholar
Finney, JL (1977) Modelling the structures of amorphous metals and alloys. Nature 266, 309314.Google Scholar
Fitting, L, Thiel, S, Schmehl, A, Mannhart, J Muller, DA (2006) Subtleties in ADF imaging and spatially resolved EELS: A case study of low-angle twist boundaries in SrTiO3 . Ultramicroscopy 106, 10531061.Google Scholar
Goodman, P (1975) A practical method of three-dimensional space-group analysis using convergent-beam electron diffraction. Acta Crystallogr A 31, 804810.Google Scholar
Hammel, M Rose, H (1993) Resolution and optimum conditions for dark-field STEM and CTEM imaging. Ultramicroscopy 49, 8186.Google Scholar
Hanwell, MD, Curtis, DE, Lonie, DC, Vandermeersch, T, Zurek, E Hutchison, GR (2012) Avogadro: An advanced semantic chemical editor, visualization, and analysis platform. J Cheminformatics 4, 17.Google Scholar
Hillyard, S, Loane, RF Silcox, J (1993) Annular dark-field imaging: Resolution and thickness effects. Ultramicroscopy 49, 1425.Google Scholar
Hovden, R Muller, DA (2012) Efficient elastic imaging of single atoms on ultrathin supports in a scanning transmission electron microscope. Ultramicroscopy 123, 5965.Google Scholar
Hovden, R, Jiang, Y, Xin, HL Kourkoutis, LF (2015) Periodic artifact reduction in Fourier transforms of full field atomic resolution images. Microsc Microanal 21, 436441.Google Scholar
Hovden, R, Tsen, AW, Liu, P, Savitzky, BH, BaggariEl, I. El, I., Liu, Y, Lu, W, Sun, Y, Kim, P, Pasupathy, AN Kourkoutis, LF (2016) Atomic lattice disorder in charge-density-wave phases of exfoliated dichalcogenides (1T-TaS2). Proc Natl Acad Sci U S A 113, 1142011424.Google Scholar
Hovden, R, Xin, HL Muller, DA (2010) Extended depth of field for high-resolution scanning transmission electron microscopy. Microsc Microanal 17, 7580.Google Scholar
Hovden, R, Xin, HL Muller, DA (2012) Channeling of a subangstrom electron beam in a crystal mapped to two-dimensional molecular orbitals. Phys Rev B 86, 195415.Google Scholar
Hsieh, S-M Colella, R (1987) Dimensional effects of Debye-Waller factors in layered crystals. Solid State Commun 63, 4750.Google Scholar
Kertesz, M Hoffmann, R (1984) Octahedral vs. trigonal-prismatic coordination and clustering in transition-metal dichalcogenides. J Am Chem Soc 106, 34533460.Google Scholar
Kirkland, EJ (2010) Advanced Computing in Electron Microscopy, 2nd ed. Boston, MA: Springer.Google Scholar
Kirkland, EJ, Loane, RF Silcox, J (1987) Simulation of annular dark field STEM images using a modified multislice method. Ultramicroscopy 23, 7796.Google Scholar
LeBeau, JM, Findlay, SD, Allen, LJ Stemmer, S (2010a) Standardless atom counting in scanning transmission electron microscopy. Nano Lett 10, 44054408.Google Scholar
LeBeau, JM, Findlay, SD, Allen, LJ Stemmer, S (2010b) Position averaged convergent beam electron diffraction: Theory and applications. Ultramicroscopy 110, 118125.Google Scholar
Loane, RF, Xu, P Silcox, J (1991) Thermal vibrations in convergent-beam electron diffraction. Acta Crystallogr A 47, 267278.Google Scholar
Lu, X, Utama, MIB, Lin, J, Luo, X, Zhao, Y, Zhang, J, Pantelides, ST, Zhou, W, Quek, SY Xiong, Q (2015) Rapid and nondestructive identification of polytypism and stacking sequences in few‐layer molybdenum diselenide by Raman spectroscopy. Adv Mater 27, 45024508.Google Scholar
Malis, T, Cheng, SC Egerton, RF (1988) EELS log‐ratio technique for specimen‐thickness measurement in the TEM. J Electron Microsc Tech 8, 193200.Google Scholar
Mkhoyan, KA, Maccagnano-Zacher, SE, Kirkland, EJ Silcox, J (2008) Effects of amorphous layers on ADF-STEM imaging. Ultramicroscopy 108, 791803.Google Scholar
Momma, K Izumi, F (2011) VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data. J Appl Crystallogr 44, 12721276.Google Scholar
Muller, DA, Edwards, B, Kirkland, EJ Silcox, J (2001) Simulation of thermal diffuse scattering including a detailed phonon dispersion curve. Ultramicroscopy 86, 371380.Google Scholar
Schönfeld, B, Huang, JJ Moss, SC (1983) Anisotropic mean-square displacements (MSD) in single-crystals of 2H- and 3R-MoS2 . Acta Crystallogr B 39, 404407.Google Scholar
Splendiani, A, Sun, L, Zhang, Y, Li, T, Kim, J, Chim, CY, Galli, G Wang, F (2010) Emerging photoluminescence in monolayer MoS2 . Nano Lett 10, 12711275.Google Scholar
Thompson, AH, Gamble, RF Revelli, JF (1971) Transitions between semiconducting and metallic phases in 1-T TaS2 . Solid State Commun 9, 981985.Google Scholar
Treacy, MMJ (2011) Z dependence of electron scattering by single atoms into annular dark-field detectors. Microsc Microanal 17, 847858.Google Scholar
Tsen, AW, Hovden, R, Wang, DZ, Kim, YD, Okamoto, J, Spoth, KA, Liu, Y, Lu, WJ, Sun, YP, Hone, J, Kourkoutis, LF, Kim, P Pasupathy, AN (2015) Structure and control of charge density waves in two-dimensional 1T-TaS2 . Proc Natl Acad Sci U S A 112, 1505415059.Google Scholar
Van den Broek, W, Rosenauer, A, Goris, B, Martinez, GT, Bals, S, Van Aert, S Van Dyck, D (2012) Correction of non-linear thickness effects in HAADF STEM electron tomography. Ultramicroscopy 116, 812.Google Scholar
Wilson, JA, Di Salvo, FJ Mahajan, S (1975) Charge-density waves and superlattices in metallic layered transition-metal dichalcogenides. Adv Phys 24, 117201.Google Scholar
Xia, M, Li, B, Yin, K, Capellini, G, Niu, G, Gong, Y, Zhou, W, Ajayan, PM Xie, Y-H (2015) Spectroscopic signatures of AA′ and AB stacking of chemical vapor deposited bilayer MoS2 . ACS Nano 9, 1224612254.Google Scholar
Xin, HL, Intaraprasonk, V Muller, DA (2008) Depth sectioning of individual dopant atoms with aberration-corrected scanning transmission electron microscopy. Appl Phys Lett 92, 013125.Google Scholar
Xin, HL, Zhu, Y Muller, DA (2012) Determining on-axis crystal thickness with quantitative position-averaged incoherent bright-field signal in an aberration-corrected STEM. Microsc Microanal 18, 720727.Google Scholar
Xu, P, Loane, RF Silcox, J (1991) Energy-filtered convergent-beam electron diffraction in STEM. Ultramicroscopy 38, 127133.Google Scholar
Yan, J, Xia, J, Wang, X, Liu, L, Kuo, J-L, Tay, BK, Chen, S, Zhou, W, Liu, Z Shen, ZX (2015) Stacking-dependent interlayer coupling in trilayer MoS2 with broken inversion symmetry. Nano Lett 15, 81558161.Google Scholar
Yu, Y, Yang, F, Lu, XF, Yan, YJ, Cho, Y-H, Ma, L, Niu, X, Kim, S, Son, Y-W, Feng, D, Li, S, Cheong, S-W, Chen, XH Zhang, Y (2015) Gate-tunable phase transitions in thin flakes of 1T-TaS2 . Nat Nanotechnol 10, 270276.Google Scholar
Zuo, JM Spence, JCH (2013) Electron Microdiffraction . New York: Springer.Google Scholar
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