REVIEW 3 major objections 4 minor 47 references
Microstructure and Elastic Constants of Transition Metal Dichalcogenide Monolayers from Friction and Shear Force Microscopy
T0 review · 3 major / 4 minor · reviewed 2026-08-14 · deepseek-v4-flash
Pith's one-line read Angle-dependent shear-force microscopy on CVD-grown WS2 monolayers yields experimental fourth-order elastic constants and a nondestructive way to map grain boundaries, crystal orientation, and strain.
desk verdict The LFM/TSM microstructure mapping is a useful, well-validated contribution, but the elastic constant extraction is underdetermined by the printed equation and should not be trusted as reported. read the letter →
The pith
A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.
The reading
What carries the argument
The load-bearing identity is Eq. (1), a linear-elastic relation previously derived for TSM that writes the transverse shear signal $T$ as a constant $G$ times a combination of the fourth-order elastic constants $C_{1111}$, $C_{3333}$, $C_{1122}$, and $C_{1133}$ multiplied by trigonometric functions of $3\theta+\alpha$, where $\theta$ is the scan angle and $\alpha$ the grain tilt. The mechanism is rotation: as the sample turns against the scan direction, the threefold symmetric lattice changes the shear stress on the tip, producing the 60°-periodic signal whose amplitude and phase are used to fit the constants. The factor $G$ is meant to absorb applied stress, cantilever-tip geometry, instrument sensitivity, and tip-sample contact area.
What would settle it
Measure the angle-dependent TSM signal on the same WS2 monolayer at two different applied loads or scan speeds; if the fitted elastic constants change, the rotation-independent $G$ premise fails. Alternatively, compare the reported $C_{1111} \approx 15000\ \mathrm{GPa}$ and $C_{3333} \approx 7000\ \mathrm{GPa}$ with independent elastic measurements of a suspended monolayer, such as nanoindentation or Brillouin scattering.
Extended reading notes
Core claim
The central discovery is that the transverse shear microscopy signal of a monolayer WS2 flake changes periodically as the flake is rotated relative to the scan direction, with a period of 60°, and that this rotation dependence can be fit by a linear-elastic relation to yield estimates of the fourth-order elastic constants. On the paper's own terms, angle-dependent TSM measurements enable the authors to acquire these elastic constants experimentally, reporting $C_{1111} \approx 15000\ \mathrm{GPa}$, $C_{3333} \approx 7000\ \mathrm{GPa}$, $C_{1122} \approx 500\ \mathrm{GPa}$, and $C_{1133} \approx -800\ \mathrm{GPa}$, with $G = 3.4\ \mathrm{mV/GPa}$. The authors also establish a contrast taxonomy: single crystals show no LFM/TSM contrast, strained grains show diffuse LFM contrast that disappears after transfer, sharp LFM lines locate grain boundaries, and TSM reveals orientation differences except for high-symmetry 120° boundaries that are invisible because of the threefold lattice symmetry.
Load-bearing premise
The quantitative claim presupposes that the measured TSM signal is a linear-elastic response described by Eq. (1) with a single factor $G$ that stays constant as the sample rotates; the derivation is placed in the Supporting Information and the paper does not verify that tip geometry, contact area, or instrument sensitivity are actually rotation-independent.
Editorial extensions
If this is right
- Rotational TSM can assign the relative crystallographic orientation of irregularly shaped flakes from the angular shift of fitted $T(\theta)$ curves, offering a nondestructive alternative to dark-field transmission electron microscopy.
- The reported $C_{1111} \approx 2C_{3333}$ and the dominance of $C_{1111}$ over $C_{1122}$ and $C_{1133}$ provide benchmark values for density-functional and continuum calculations of WS2 monolayer elasticity.
- Combining LFM and TSM distinguishes single-grain from multi-grain flakes even when TSM alone is ambiguous, because 120° twin boundaries are invisible to TSM under the threefold symmetry.
- Because the contrast mechanism is elastic anisotropy, the same LFM/TSM protocol should apply to other monolayer TMDCs, and the paper demonstrates the approach on CVD-grown MoS2 as well.
- Angle-dependent TSM can also reveal minimal grain misorientation, giving quantitative statistics on how neighboring domains are tilted within a flake.
Reading between the lines
- A natural extension, not stated in the paper, is to vary the applied load or scan speed during angle-dependent TSM; if the fitted constants change, the assumption that $G$ is rotation-independent would need revision.
- The extracted constants concern in-plane shear stiffness, so connecting $C_{1111} \approx 2C_{3333}$ to conventional in-plane Young's moduli would require a separate elasticity model relating monolayer stiffness to the measured transverse shear response.
- The same rotational protocol could be applied to map local orientation fields grain-by-grain over large CVD films, producing statistics on grain-boundary misorientation distributions that growth models could be checked against.
Signed reviews
Editorial analysis
A structured set of objections, weighed in public.
Referee Report
Summary. The manuscript reports a combined lateral force microscopy (LFM) and transverse shear microscopy (TSM) study of CVD-grown WS2 monolayers. It demonstrates that LFM can reveal strain fields and grain boundaries, and that TSM can reveal relative crystallographic orientation, with support from PL mapping, transfer experiments, and SAED. The authors further claim that angle-dependent TSM measurements allow the experimental determination of the fourth-order elastic constants of monolayer WS2, reporting C1111 ≈ 15000 GPa, C3333 ≈ 7000 GPa, C1122 ≈ 500 GPa, and C1133 ≈ −800 GPa, with a scale factor G = 3.4 mV/GPa and the relation C1111 ≈ 2C3333.
Significance. The microstructure characterization part is significant: the combined LFM/TSM approach is non-destructive, rapid, and large-area, and the paper provides a useful table of expected contrasts for different microstructures. The evidence for grain boundary identification (sharp line contrast persisting after transfer, corresponding PL quenching, agreement with SAED) is compelling. If the elastic constant extraction were valid, it would be the first experimental determination of fourth-order elastic constants of monolayer TMDCs and thus of substantial interest. However, as detailed below, the elastic constant extraction from Eq. (1) is underdetermined, so the quantitative claim is not supported.
major comments (3)
- [Eq. (1), Section 'Elastic constants of WS2'] The displayed Eq. (1) is underdetermined for the claimed parameters. Let A = cos(3θ+α) sin^4(3θ+α) − cos^4(3θ+α) sin(3θ+α). The first three elastic-constant terms are C1111 A, C4444 (−2A), and C1122 (−A), so they collapse into a single coefficient G(C1111 − 2C4444 − C1122) multiplying A. Only the fourth term, C1133 [cos^9(3θ+α) − sin^9(3θ+α)], is an independent angular function. A rotation scan therefore constrains at most two combinations of the five unknowns (C1111, C4444, C1122, C1133, G), so the individual reported values are not identifiable from the data. The 'good agreement' in Fig. 6d is a back-fit, not an independent validation.
- [Eq. (1) and reported fit values] There is an inconsistency between Eq. (1) and the reported constants. The equation contains C1111, C4444, C1122, and C1133, whereas the text reports fitted values for C1111, C3333, C1122, and C1133, with no value given for C4444 and no C3333 appearing in the model. Additionally, the derivation of Eq. (1) is placed in the Supporting Information, which is not included in the submitted manuscript, so the assumptions (linear-elastic response, rotation-independent G, hexagonal symmetry reduction) cannot be checked. The authors must provide the full derivation or clearly state any symmetry relations that reduce the number of independent constants.
- [Figure 6d, sensitivity analysis] The sensitivity analysis in Fig. 6d does not support the claimed constraints. Varying C1111 or C3333 while keeping the other constants fixed changes the curve in a way that can be compensated by adjusting the unidentifiable combination G(C1111 − 2C4444 − C1122) and G, so the dashed lines do not demonstrate that the data are sensitive to the individual constants. Furthermore, the paper's caveat about the unknown G only addresses absolute values; the relative relations C1111 ≈ 2C3333, C1111 >> C1122, and C1111 >> C1133 are not established because they rely on the same unidentifiable decomposition.
minor comments (4)
- [General] The manuscript contains placeholder text for the DOI and 'Received' lines that should be completed.
- [References] Reference [46] in the text is cited as the source of the TSM relation, but the reference list assigns [46] to a different paper than [47]; please verify the citation intention.
- [Eq. (1) notation] The elastic-constant labels in Eq. (1) (C&&&&, C&&88, C&&44) are garbled and should be typeset unambiguously as C1111, C1122, etc., with a definition of the index convention for a two-dimensional crystal.
- [Periodicity, Section 'Elastic constants of WS2'] The text states that the measured TSM signal has a 60° periodicity, while the functional form in Eq. (1) depends on cos(3θ+α) and sin(3θ+α), which have 120° periodicity; the relationship between the model and the observed periodicity should be clarified.
Circularity Check
The reported WS2 elastic constants are best-fit outputs of an underdetermined angular model; the 'good agreement' is a back-check of the fit, not an independent prediction.
-
fitted input called prediction
[This claim appears in the paragraph after Eq. (1) in the 'Elastic constants of WS2' section, describing Fig. 6d.]
"A subsequent fitting (solid lines in Figure 6d) exhibits good agreement with the measured TSM data for elastic constants of C1111 ≈ 15000 GPa, C3333 ≈ 7000 GPa, C1122 ≈ 500 GPa and C1133 ≈ −800 GPa."
The solid lines are Eq. (1) evaluated at the constants obtained by that same fitting. The agreement is therefore the least-squares objective restated as a result; any fit will show good agreement by construction. The abstract's claim that angle-dependent TSM measurements 'acquire' the constants uses this back-check as support, but it is not a test against independent data or an external benchmark.
-
other
[The printed model is Eq. (1) in the 'Elastic constants of WS2' section.]
"𝑇=𝐺{𝐶&&&&[cos(3𝜃+𝛼)∙sin4(3𝜃+𝛼)−cos4(3𝜃+𝛼)∙sin(3𝜃+𝛼)]+𝐶4444[2cos4(3𝜃+𝛼)∙sin(3𝜃+𝛼)−2cos(3𝜃+𝛼)∙sin4(3𝜃+𝛼)]+𝐶&&88[cos4(3𝜃+𝛼)∙sin(3𝜃+𝛼)−cos(3𝜃+𝛼)∙sin4(3𝜃+𝛼)]+𝐶&&44[cos9(3𝜃+𝛼)−sin9(3𝜃+𝛼)]} (1)"
In the printed equation, writing c = cos(3θ+α) and s = sin(3θ+α), the second angular bracket is exactly -2 times the first and the third is exactly -1 times the first; hence the first three elastic-constant terms collapse into a single angular function. A one-dimensional angle sweep with unknown multiplicative G therefore determines at most two independent combinations of the four reported Cijkl, while five parameters are reported. The individual constants and the emphasized relation C1111 ≈ 2C3333 are not fixed by the data; they are carried over from the MoS2 DFT initial guess along the unconstrained directions. The claimed extraction of elastic constants thus reduces to the fitting ansatz and initial guess by construction.
full rationale
The microstructure part of the paper is self-contained: LFM/TSM contrast is interpreted using a borrowed, independently published model and is cross-checked by PL mapping, transfer experiments, and electron diffraction. The elastic-constant portion, however, is the central quantitative claim and is circular in two related senses. First, the 'good agreement' in Fig. 6d is a back-check of the fit: the solid lines are generated from Eq. (1) with the very parameters just fitted, so the agreement is not an independent prediction. Second, the printed Eq. (1) is underdetermined as written: the first three angular brackets are proportional, leaving only two independent angular functions to constrain five unknowns (four Cijkl plus G). The paper itself concedes that 'the obtained absolute values are not unambiguous due to the unknown constant G,' but the printed equation shows a stronger degeneracy: even with G fixed, the constants enter through only two independent combinations. The reported values and the robust relation C1111 ≈ 2C3333 are therefore not uniquely determined by the experiment; they depend on the MoS2 DFT starting values along the flat directions of the fit. This is a mathematical identifiability failure visible in the paper's own equation, not a dispute about consensus. The absent Supporting Information derivation, which the paper cites for Eq. (1), prevents checking whether a fuller model removes the proportionality; on the printed evidence, the elastic constants are best-fit outputs rather than independently acquired material properties. These problems do not affect the grain-boundary/orientation imaging conclusions, which have independent support.
Assumptions & free parameters
free parameters (5)
- C1111 =
≈15000 GPa
- C3333 =
≈7000 GPa
- C1122 =
≈500 GPa
- C1133 =
≈−800 GPa
- G =
3.4 mV/GPa
assumptions (4)
- domain assumption Equation (1) from Kalihari et al. correctly describes the TSM signal as a function of elastic constants and rotation angle for a hexagonal monolayer
- domain assumption The scale factor G is constant during rotation
- domain assumption The monolayer has hexagonal symmetry with threefold rotation, so the TSM signal has 60° periodicity
- domain assumption The tilt angle α measured from flake edges equals the crystallographic misorientation between grains
Cite this review
Pith. "Pith review of Microstructure and Elastic Constants of Transition Metal Dichalcogenide Monolayers from Friction and Shear Force Microscopy." pith.science (2026). https://pith.science/paper/6I4UGLRH
@misc{pith2026190807843,
author = {Pith},
title = {Pith review of: Microstructure and Elastic Constants of Transition Metal Dichalcogenide Monolayers from Friction and Shear Force Microscopy},
year = {2026},
howpublished = {\url{https://pith.science/paper/6I4UGLRH}},
note = {Machine review of arXiv:1908.07843}
}
read the original abstract
Optical and electrical properties of two-dimensional transition metal dichalcogenides (TMDCs) grown by chemical vapor deposition (CVD) are strongly determined by their microstructure. Consequently, the visualization of spatial structural variations is of paramount importance for future applications. Here we demonstrate how grain boundaries, crystal orientation, and strain fields can unambiguously be identified with combined lateral force microscopy (LFM) and transverse shear microscopy (TSM) for CVD-grown tungsten disulfide (WS2) monolayers, on length scales that are relevant for optoelectronic applications. Further, angle-dependent TSM measurements enable us to acquire the fourth-order elastic constants of monolayer WS2 experimentally. Our results facilitate high-throughput and nondestructive microstructure visualization of monolayer TMDCs, insights into their elastic properties, thus providing an accessible tool to support the development of advanced optoelectronic devices based on such two-dimensional semiconductors.
Figures
Figures from the paper (3 more)
Reference graph
Works this paper leans on
-
[1]
Kirchhof, Andreas Opitz, Christoph T
1 DOI: 10.1002/((please add manuscript number)) Communication Microstructure and Elastic Constants of Transition Metal Dichalcogenide Monolayers from Friction and Shear Force Microscopy Xiaomin Xu†, Thorsten Schultz†, Ziyu Qin, Nikolai Severin, Benedikt Haas, Sumin Shen, Jan N. Kirchhof, Andreas Opitz, Christoph T. Koch, Kirill Bolotin, Jürgen P. Rabe, Go...
-
[2]
S. Manzeli, D. Ovchinnikov, D. Pasquier, O. V . Yazyev, A. Kis, Nat. Rev. Mater . 2017, 2, 17033
work page 2017
-
[3]
K. F. Mak, C. Lee, J. Hone, J. Shan, T. F. Heinz, Phys. Rev. Lett. 2010, 105, 136805
work page 2010
-
[4]
A. Splendiani, L. Sun, Y . Zhang, T. Li, J. Kim, C.-Y . Chim, G. Galli, F. Wang, Nano Lett. 2010, 10,
work page 2010
-
[5]
Q. H. Wang, K. Kalantar-Zadeh, A. Kis, J. N. Coleman, M. S. Strano, Nat. Nanotechnol. 2012, 7,
work page 2012
- [6]
-
[7]
F. H. L. Koppens, T. Mueller, P. Avouris, A. C. Ferrari, M. S. Vitiello, M. Polini, Nat. 15 Nanotechnol. 2014, 9,
work page 2014
-
[8]
O. Lopez-Sanchez, D. Lembke, M. Kayci, A. Radenovic, A. Kis, Nat. Nanotechnol. 2013, 8,
work page 2013
Show all 47 references
-
[9]
K. F. Mak, J. Shan, Nat. Photonics 2016, 10,
2016
-
[10]
Z. Sun, A. Martinez, F. Wang, Nat. Photonics 2016, 10,
2016
-
[11]
Y . Lee, X. Zhang, W. Zhang, M. Chang, C. Lin, K. Chang, Y . Y u, J. T. Wang, C. Chang, L. Li, T. Lin, Adv. Mater . 2018, 24,
2018
-
[12]
Y . Zhan, Z. Liu, S. Najmaei, P. M. Ajayan, J. Lou, Small 2016, 8,
2016
-
[14]
J. Zhou, J. Lin, X. Huang, Y . Zhou, Y . Chen, J. Xia, H. Wang, Y . Xie, H. Y u, J. Lei, D. Wu, F. Liu, Q. Fu, Q. Zeng, C.-H. Hsu, C. Yang, L. Lu, T. Y u, Z. Shen, H. Lin, B. I. Yakobson, Q. Liu, K. Suenaga, G. Liu, Z. Liu, Nature 2018, 556,
2018
-
[15]
Li, Y .-C
S. Li, Y .-C. Lin, W. Zhao, J. Wu, Z. Wang, Z. Hu, Y . Shen, D.-M. Tang, J. Wang, Q. Zhang, H. Zhu, L. Chu, W. Zhao, C. Liu, Z. Sun, T. Taniguchi, M. Osada, W. Chen, Q.-H. Xu, A. T. S. Wee, K. Suenaga, F. Ding, G. Eda, Nat. Mater . 2018, 17,
2018
-
[16]
H. Liu, J. Lu, K. Ho, Z. Hu, Z. Dang, A. Carvalho, H. R. Tan, E. S. Tok, C. H. Sow, Nano Lett. 2016, 16,
2016
-
[17]
Sheng, X
Y . Sheng, X. Wang, K. Fujisawa, S. Ying, A. L. Elias, Z. Lin, W. Xu, Y . Zhou, A. M. Korsunsky, H. Bhaskaran, M. Terrones, J. H. Warner, ACS Appl. Mater . Interfaces 2017, 9, 15005
2017
-
[19]
Q. Ji, Y . Zhang, Y . Zhang, Z. Liu, Chem. Soc. Rev. 2015, 44,
2015
-
[20]
J. Wang, H. Y u, X. Zhou, X. Liu, R. Zhang, Z. Lu, J. Zheng, L. Gu, K. Liu, D. Wang, L. Jiao, Nat. Commun. 2017, 8,
2017
-
[21]
A. M. van der Zande, P . Y . Huang, D. A. Chenet, T. C. Berkelbach, Y . You, G.-H. Lee, T. F. Heinz, D. R. Reichman, D. A. Muller, J. C. Hone, Nat. Mater . 2013, 12,
2013
-
[22]
Najmaei, Z
S. Najmaei, Z. Liu, W. Zhou, X. Zou, G. Shi, S. Lei, B. I. Yakobson, J.-C. Idrobo, P. M. Ajayan, J. Lou, Nat. Mater . 2013, 12,
2013
-
[23]
Z. Liu, M. Amani, S. Najmaei, Q. Xu, X. Zou, W. Zhou, T. Y u, C. Qiu, A. G. Birdwell, F. J. Crowne, R. V ajtai, B. I. Yakobson, Z. Xia, M. Dubey, P. M. Ajayan, J. Lou, Nat. Commun. 2014, 5,
2014
-
[24]
Zhang, Y
Y. Zhang, Y . Zhang, Q. Ji, J. Ju, H. Y uan, J. Shi, T. Gao, D. Ma, M. Liu, Y . Chen, X. Song, H. Y . Hwang, Y . Cui, Z. Liu, ACS Nano 2013, 7,
2013
-
[25]
Y . Rong, K. He, M. Pacios, A. W. Robertson, H. Bhaskaran, J. H. Warner, ACS Nano 2015, 9,
2015
-
[26]
J. Wang, X. Xu, R. Qiao, J. Liang, C. Liu, B. Zheng, L. Liu, P . Gao, Q. Jiao, D. Y u, Y . Zhao, K. Liu, Nano Res. 2018, DOI: 10.1007/s12274-018-1991-2
2018 doi
-
[27]
X. Yin, Z. Ye, D. A. Chenet, Y . Ye, K. O’Brien, J. C. Hone, X. Zhang, Science 2014, 344,
2014
-
[28]
Karvonen, A
L. Karvonen, A. Säynätjoki, M. J. Huttunen, A. Autere, B. Amirsolaimani, S. Li, R. A. Norwood, N. Peyghambarian, H. Lipsanen, G. Eda, K. Kieu, Z. Sun, Nat. Commun. 2017, 8, 15714
2017
-
[29]
Kasas, G
S. Kasas, G. Longo, G. Dietler, J. Phys. D: Appl. Phys. 2013, 46, 133001
2013
-
[30]
Kalihari, E
V . Kalihari, E. B. Tadmor, G. Haugstad, C. D. Frisbie, Adv. Mater. 2008, 20,
2008
-
[31]
J. S. Choi, J.-S. Kim, I.-S. Byun, D. H. Lee, M. J. Lee, B. H. Park, C. Lee, D. Yoon, H. Cheong, K. H. Lee, Y .-W. Son, J. Y . Park, M. Salmeron, Science 2011, 333,
2011
-
[32]
M. Li, J. Shi, L. Liu, P. Y u, N. Xi, Y . Wang, Sci. Technol. Adv. Mater . 2016, 17,
2016
-
[33]
H. R. Gutiérrez, N. Perea-López, A. L. Elías, A. Berkdemir, B. Wang, R. Lv, F. López-Urías, V . H. Crespi, H. Terrones, M. Terrones, Nano Lett. 2013, 13,
2013
-
[34]
C. Cong, J. Shang, X. Wu, B. Cao, N. Peimyoo, C. Qiu, L. Sun, T. Y u, Adv. Optical Mater. 2014, 2,
2014
-
[35]
Carozo, Y
V. Carozo, Y. Wang, K. Fujisawa, B. R. Carvalho, A. McCreary, S. Feng, Z. Lin, C. Zhou, N. Perea-López, A. L. Elías, B. Kabius, V. H. Crespi, M. Terrones, Sci. Adv. 2017, 3, e1602813
2017
-
[36]
W. H. Chae, J. D. Cain, E. D. Hanson, A. A. Murthy, V . P . Dravid, Appl. Phys. Lett. 2017, 111, 143106
2017
-
[37]
H. J. Conley, B. Wang, J. I. Ziegler, R. F. Haglund, S. T. Pantelides, K. I. Bolotin, Nano Lett. 2013, 13,
2013
-
[38]
W. Bao, N. J. Borys, C. Ko, J. Suh, W. Fan, A. Thron, Y . Zhang, A. Buyanin, J. Zhang, S. Cabrini, P . D. Ashby, A. Weber-Bargioni, S. Tongay, S. Aloni, D. F. Ogletree, J. Wu, M. B. Salmeron, P . J. Schuck, Nat. Commun. 2015, 6,
2015
-
[39]
Alharbi, D
A. Alharbi, D. Shahrjerdi, Appl. Phys. Lett. 2016, 109, 193502
2016
-
[40]
M. R. Rosenberger, H.-J. Chuang, K. M. McCreary, C. H. Li, B. T. Jonker, ACS Nano 2018, 12,
2018
-
[41]
Govind Rajan, J
A. Govind Rajan, J. H. Warner, D. Blankschtein, M. S. Strano, ACS Nano 2016, 10,
2016
-
[42]
H. Li, Y . Li, A. Aljarb, Y . Shi, L.-J. Li, Chem. Rev. 2017, DOI: 10.1021/acs.chemrev. 7b00212
2017 doi
-
[43]
X. Liu, I. Balla, H. Bergeron, M. C. Hersam, J. Phys. Chem. C 2016, 120, 20798
2016
-
[44]
Komsa, A
H.-P. Komsa, A. V . Krasheninnikov, Adv. Electron. Mater. 2017, 3, 1600468
2017
-
[45]
Cheng, T
J. Cheng, T. Jiang, Q. Ji, Y . Zhang, Z. Li, Y . Shan, Y . Zhang, X. Gong, W. Liu, S. Wu, Adv. Mater . 2015, 27,
2015
-
[46]
S. Park, M. S. Kim, H. Kim, J. Lee, G. H. Han, J. Jung, J. Kim, ACS Nano 2015, 9, 11042
2015
-
[47]
Kalihari, G
V . Kalihari, G. Haugstad, C. D. Frisbie, Phys. Rev. Lett. 2010, 104, 169905
2010
-
[48]
Q. Peng, S. De, Phys. Chem. Chem. Phys. 2013, 15, 19427
2013
-
[50]
C. Luo, C. Wang, X. Wu, J. Zhang, J. Chu, Small 2017, 13, 1604259. Table
2017
Reviewed August 14, 2026 · model on record in the stance chip above.
Discussion (0). Continue with ORCID to comment.