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Contrasting impurity-induced magnetism and dynamics in 2H−MoTe2

Jonas A. Krieger1,*,†, Igor P. Rusinov2, Sourabh Barua3,‡, Aris Chatzichristos4,5, Jared Croese6, Derek Fujimoto4,5,§, Stefan Holenstein1,7, Victoria L. Karner5,8, Ryan M. L. McFadden5,8,§ et al.

John O. Ticknor5,8, W. Andrew MacFarlane5,8,9, Robert F. Kiefl4,5,9, Geetha Balakrishnan3, Evgueni V. Chulkov10,11,12, Stuart S. P. Parkin13, and Zaher Salman1,∥

  • *Contact author: jonas.krieger@psi.ch
  • †Formerly at Max Planck Institut für Mikrostrukturphysik, Weinberg 2, 06120 Halle, Germany.
  • ‡Present address: Department of Physics, Central University of Punjab, Bathinda 151401, India.
  • §Present address: TRIUMF, Vancouver, British Columbia V6T 2A3, Canada.
  • ∥Contact author: zaher.salman@psi.ch
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Phys. Rev. Research 8, 023316 – Published 18 June, 2026

DOI: https://doi.org/10.1103/49q2-5vl8

Abstract

We investigate the behavior of interstitial Li+8 implanted near the surface of 2H−MoTe2 using β-detected nuclear magnetic resonance. We find that, unlike the muon, Li+8 does not show any signature of induced magnetism. This result is consistent with density functional theory, which identifies the Li stopping site at the 2a Wyckoff position in the van der Waals gap and confirms the absence of detectable Li-induced electronic spin polarization. Both the spin-lattice relaxation and the resonance line shape show evidence of pronounced spin dynamics above ∼200K, reminiscent of local stochastic Li+8 motion within a cage. The resonance line shape consists of quadrupolar satellites on top of a broad central peak. To better understand the interaction of Li+8 with the host material, we employ a frequency-comb measurement by simultaneously exciting four frequencies corresponding to the first-order quadrupolar satellite transitions, ν0±3νcomb and ν0±νcomb, around the Larmor frequency ν0 as a function of νcomb. This offers an enhanced sensitivity to the quadrupolar split portion of the line. Using this method, we find a small decrease in the quadrupolar frequency with increasing temperature, showing the typical behavior associated with thermally excited phonons and the absence of any magnetic response, in contrast to what was observed for other defects in 2H−MoTe2.

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References (52)

  1. S. Manzeli, D. Ovchinnikov, D. Pasquier, O. V. Yazyev, and A. Kis, 2D transition metal dichalcogenides, Nat. Rev. Mater. 2, 17033 (2017).
  2. A. K. Geim and I. V. Grigorieva, Van der Waals heterostructures, Nature (London) 499, 419 (2013).
  3. C. R. Rajamathi, U. Gupta, N. Kumar, H. Yang, Y. Sun, V. Süß, C. Shekhar, M. Schmidt, H. Blumtritt, P. Werner, B. Yan, S. Parkin, C. Felser, and C. N. R. Rao, Weyl semimetals as hydrogen evolution catalysts, Adv. Mater. 29, 1606202 (2017).
  4. A. J. Grant, T. M. Griffiths, G. D. Pitt, and A. D. Yoffe, The electrical properties and the magnitude of the indirect gap in the semiconducting transition metal dichalcogenide layer crystals, J. Phys. C: Solid State Phys. 8, L17 (1975).
  5. A. Conan, D. Delaunay, A. Bonnet, A. G. Moustafa, and M. Spiesser, Temperature dependence of the electrical conductivity and thermoelectric power in MoTe2 single crystals, Phys. Status Solidi B 94, 279 (1979).
  6. I. G. Lezama, A. Ubaldini, M. Longobardi, E. Giannini, C. Renner, A. B. Kuzmenko, and A. F. Morpurgo, Surface transport and band gap structure of exfoliated 2H−MoTe2 crystals, 2D Mater. 1, 021002 (2014).
  7. H. Xu, S. Fathipour, E. W. Kinder, A. C. Seabaugh, and S. K. Fullerton-Shirey, Reconfigurable ion gating of 2H−MoTe2 field-effect transistors using poly(ethylene oxide)-CsClO4 solid polymer electrolyte, ACS Nano 9, 4900 (2015).
  8. Y. Ding, N. Zhou, L. Gan, X. Yan, R. Wu, I. H. Abidi, A. Waleed, J. Pan, X. Ou, Q. Zhang, M. Zhuang, P. Wang, X. Pan, Z. Fan, T. Zhai, and Z. Luo, Stacking-mode confined growth of 2H−MoTe2/MoS2 bilayer heterostructures for UV-vis-IR photodetectors, Nano Energy 49, 200 (2018).
  9. G. Li, Y. Xu, Z. Song, Q. Yang, Y. Zhang, J. Liu, U. Gupta, V. Süß, Y. Sun, P. Sessi, S. S. P. Parkin, B. A. Bernevig, and C. Felser, Obstructed surface states as the descriptor for predicting catalytic active sites in inorganic crystalline materials, Adv. Mater. 34, 2201328 (2022).
  10. Z. Guguchia, A. Kerelsky, D. Edelberg, S. Banerjee, F. von Rohr, D. Scullion, M. Augustin, M. Scully, D. A. Rhodes, Z. Shermadini, et al., Magnetism in semiconducting molybdenum dichalcogenides, Sci. Adv. 4, eaat3672 (2018).
  11. Y. Ma, Y. Dai, M. Guo, C. Niu, J. Lu, and B. Huang, Electronic and magnetic properties of perfect, vacancy-doped, and nonmetal adsorbed MoSe2, MoTe2 and WS2 monolayers, Phys. Chem. Chem. Phys. 13, 15546 (2011).
  12. H. González-Herrero, J. M. Gómez-Rodríguez, P. Mallet, M. Moaied, J. J. Palacios, C. Salgado, M. M. Ugeda, J.-Y. Veuillen, F. Yndurain, and I. Brihuega, Atomic-scale control of graphene magnetism by using hydrogen atoms, Science 352, 437 (2016).
  13. J. A. Krieger, D. Tay, I. P. Rusinov, S. Barua, P. K. Biswas, L. Korosec, T. Prokscha, T. Schmitt, N. B. M. Schröter, T. Shang, T. Shiroka, A. Suter, G. Balakrishnan, E. V. Chulkov, V. N. Strocov, and Z. Salman, Hydrogen-impurity-induced unconventional magnetism in semiconducting molybdenum ditelluride, Phys. Rev. Mater. 7, 044414 (2023).
  14. Z. Lin, B. R. Carvalho, E. Kahn, R. Lv, R. Rao, H. Terrones, M. A. Pimenta, and M. Terrones, Defect engineering of two-dimensional transition metal dichalcogenides, 2D Mater. 3, 022002 (2016).
  15. H. Li, C. Tsai, A. L. Koh, L. Cai, A. W. Contryman, A. H. Fragapane, J. Zhao, H. S. Han, H. C. Manoharan, F. Abild-Pedersen, J. K. Nørskov, and X. Zheng, Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies, Nat. Mater. 15, 48 (2016).
  16. S. McDonnell and P. Reinke, Defects in transition metal dichalcogenides, in Defects in Two-Dimensional Materials, Materials Today, edited by R. Addou and L. Colombo (Elsevier, Amsterdam, Netherlands, 2022), Chap. 4, pp. 89–117.
  17. Z. Guguchia, F. von Rohr, Z. Shermadini, A. T. Lee, S. Banerjee, A. R. Wieteska, C. A. Marianetti, B. A. Frandsen, H. Luetkens, Z. Gong, et al., Signatures of the topological s+− superconducting order parameter in the type-II Weyl semimetal Td−MoTe2, Nat. Commun. 8, 1082 (2017).
  18. Z. Salman, R. F. Kiefl, K. H. Chow, M. D. Hossain, T. A. Keeler, S. R. Kreitzman, C. D. P. Levy, R. I. Miller, T. J. Parolin, M. R. Pearson, H. Saadaoui, J. D. Schultz, M. Smadella, D. Wang, and W. A. MacFarlane, Near-surface structural phase transition of SrTiO3 studied with zero-field β-detected nuclear spin relaxation and resonance, Phys. Rev. Lett. 96, 147601 (2006).
  19. G. D. Morris, W. A. MacFarlane, K. H. Chow, Z. Salman, D. J. Arseneau, S. Daviel, A. Hatakeyama, S. R. Kreitzman, C. D. P. Levy, R. Poutissou, R. H. Heffner, J. E. Elenewski, L. H. Greene, and R. F. Kiefl, Depth-controlled β-NMR of Li8 in a thin silver film, Phys. Rev. Lett. 93, 157601 (2004).
  20. G. D. Morris, β-NMR, Hyperfine Interact. 225, 173 (2014).
  21. C. D. P. Levy, M. R. Pearson, R. F. Kiefl, E. Mané, G. D. Morris, and A. Voss, Laser polarization facility, Hyperfine Interact. 225, 165 (2014).
  22. W. A. MacFarlane, Implanted-ion βNMR: A new probe for nanoscience, Solid State Nucl. Magn. Reson. 68–69, 1 (2015).
  23. W. A. MacFarlane, Status and progress of ion-implanted βNMR at TRIUMF, Z. Phys. Chem. 236, 757 (2022).
  24. A. Hatakeyama, Y. Hirayama, J. A. Behr, H. Izumi, C. D. P. Levy, D. Melconian, and T. Shimoda, Optical pumping at the ISAC polarizer, in Polarized Sources and Targets, edited by V. P. Derenchuk and B. von Przewoski (World Scientific, Singapore, 2002), pp. 339–343.
  25. W. Eckstein, in Computer Simulation of Ion-Solid Interactions, edited by U. Gonser, A. Mooradian, R. M. Osgood, M. B. Panish, H. Sakaki, and H. K. V. Lotsch, Springer Series in Materials Science (Springer-Verlag, Berlin, 1991).
  26. T. Minamisono, T. Ohtsubo, S. Fukuda, I. Minami, Y. Nakayama, M. Fukuda, K. Matsuta, and Y. Nojiri, New nuclear quadrupole resonance technique in β-NMR, Hyperfine Interact. 80, 1315 (1993).
  27. J. R. Adelman, D. Fujimoto, M. H. Dehn, S. R. Dunsiger, V. L. Karner, C. D. P. Levy, R. Li, I. McKenzie, R. M. L. McFadden, G. D. Morris, M. R. Pearson, M. Stachura, E. Thoeng, J. O. Ticknor, N. Ohashi, K. M. Kojima, and W. A. MacFarlane, Nuclear magnetic resonance of Li8 ions implanted in ZnO, Phys. Rev. B 106, 035205 (2022).
  28. H. J. Stöckmann, H. Ackermann, D. Dubbers, M. Grupp, and P. Heitjans, Elektrische quadrupolwechselwirkungen von F20 im MgF2-einkristall, Z. Phys. 269, 47 (1974).
  29. H. Ackermann, D. Dubbers, M. Grupp, P. Heitjans, G. Z. Putlitz, and H. J. Stöckmann, Static electric quadrupole interaction of the β-emitter F20 produced by capture of polarized neutrons in MgF2 single crystals, Phys. Lett. B 41, 143 (1972).
  30. A. Suter and B. M. Wojek, Musrfit: A free platform-independent framework for μSR data analysis, Phys. Proc. 30, 69 (2012).
  31. G. Henkelman and H. Jónsson, Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points, J. Chem. Phys. 113, 9978 (2000).
  32. T. Ozaki, Variationally optimized atomic orbitals for large-scale electronic structures, Phys. Rev. B 67, 155108 (2003).
  33. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  34. G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
  35. G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999).
  36. K. Momma and F. Izumi, VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data, J. Appl. Cryst. 44, 1272 (2011).
  37. J. S. Möller, D. Ceresoli, T. Lancaster, N. Marzari, and S. J. Blundell, Quantum states of muons in fluorides, Phys. Rev. B 87, 121108(R) (2013).
  38. F. Bernardini, P. Bonfà, S. Massidda, and R. De Renzi, Ab initio strategy for muon site assignment in wide band gap fluorides, Phys. Rev. B 87, 115148 (2013).
  39. J. Shuai, H. D. Yoo, Y. Liang, Y. Li, Y. Yao, and L. C. Grabow, Density functional theory study of Li, Na, and Mg intercalation and diffusion in MoS2 with controlled interlayer spacing, Mater. Res. Express 3, 064001 (2016).
  40. A. N. Enyashin and G. Seifert, Density-functional study of LixMoS2 intercalates (0≤x≤1), Comput. Theor. Chem. 999, 13 (2012).
  41. M. R. Panda, R. Gangwar, D. Muthuraj, S. Sau, D. Pandey, A. Banerjee, A. Chakrabarti, A. Sagdeo, M. Weyland, M. Majumder, Q. Bao, and S. Mitra, High performance lithium-ion batteries using layered 2H−MoTe2 as anode, Small 16, 2002669 (2020).
  42. J. Christiansen, P. Heubes, R. Keitel, W. Klinger, W. Loeffler, W. Sandner, and W. Witthuhn, Temperature dependence of the electric field gradient in noncubic metals, Z. Phys. B 24, 177 (1976).
  43. A. V. Nikolaev, N. M. Chtchelkatchev, D. A. Salamatin, and A. V. Tsvyashchenko, Towards an ab initio theory for the temperature dependence of electric field gradients in solids: Application to hexagonal lattices of Zn and Cd, Phys. Rev. B 101, 064310 (2020).
  44. For example, a stretched exponential A(t)=A0e−(t/T1)β fails, because the stretching coefficient β converges to nonphysical values of β∼0.2.
  45. R. M. L. McFadden, A. Chatzichristos, K. H. Chow, D. L. Cortie, M. H. Dehn, D. Fujimoto, M. D. Hossain, H. Ji, V. L. Karner, R. F. Kiefl, C. D. P. Levy, R. Li, I. McKenzie, G. D. Morris, O. Ofer, M. R. Pearson, M. Stachura, R. J. Cava, and W. A. MacFarlane, Ionic and electronic properties of the topological insulator Bi2Te2Se investigated via β-detected nuclear magnetic relaxation and resonance of Li8, Phys. Rev. B 99, 125201 (2019).
  46. W. A. MacFarlane, R. M. L. McFadden, S. L. Spencer, A. Chatzichristos, J. O. Ticknor, D. L. Cortie, M. H. Dehn, S. R. Dunsiger, D. Fujimoto, Z. H. Jang, V. L. Karner, R. F. Kiefl, G. D. Morris, and M. Stachura, Lithium ion dynamics in synthetic quartz studied via the NMR of implanted Li+8, Phys. Rev. B 112, 014103 (2025).
  47. D. Wang, M. D. Hossain, Z. Salman, D. Arseneau, K. H. Chow, S. Daviel, T. A. Keeler, R. F. Kiefl, S. R. Kreitzman, C. D. P. Levy, G. D. Morris, R. I. Miller, W. A. MacFarlane, T. J. Parolin, and H. Saadaoui, β-detected NMR of Li8 in the normal state of 2H−NbSe2, Phys. B 374, 239 (2006).
  48. R. M. L. McFadden, A. Chatzichristos, D. L. Cortie, D. Fujimoto, Y. S. Hor, H. Ji, V. L. Karner, R. F. Kiefl, C. D. P. Levy, R. Li, I. McKenzie, G. D. Morris, M. R. Pearson, M. Stachura, R. J. Cava, and W. A. MacFarlane, Local electronic and magnetic properties of the doped topological insulators Bi2Se3:Ca and Bi2Te3:Mn investigated using ion-implanted Li8β-NMR, Phys. Rev. B 102, 235206 (2020).
  49. J. Ticknor, Ion-implanted Li8 nuclear magnetic resonance study of van der Waals layered materials, Ph.D. thesis, University of British Columbia, Vancouver, Canada, 2025, https://doi.org/10.14288/1.0447683.
  50. D. L. Cortie, T. Buck, M. H. Dehn, V. L. Karner, R. F. Kiefl, C. D. P. Levy, R. M. L. McFadden, G. D. Morris, I. McKenzie, M. R. Pearson, X. L. Wang, and W. A. MacFarlane, β-NMR investigation of the depth-dependent magnetic properties of an antiferromagnetic surface, Phys. Rev. Lett. 116, 106103 (2016).
  51. J. O. Ticknor, I. Umegaki, R. M. L. McFadden, A. Chatzichristos, D. Fujimoto, V. L. Karner, R. F. Kiefl, S. Kobayashi, C. D. P. Levy, R. Li, G. D. Morris, M. R. Pearson, K. Yoshimura, J. Sugiyama, and W. A. MacFarlane, Investigation of ionic and anomalous magnetic behavior in CrSe2 using Li8β-NMR, RSC Adv. 10, 8190 (2020).
  52. J. A. Krieger, Doping and interface effects in topological materials, Ph.D. thesis, ETH Zurich, 2020, https://doi.org/10.3929/ethz-b-000460760.

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Phys. Rev. Research 8, 023316– Published 18 June, 2026
  • Received 27 January 2026
  • Accepted 22 May 2026
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