Native defects and impurities in talcum quasi-2D layers
Source abstract
Abstract
Layered semiconductors have recently emerged as capable host materials for novel quantum applications ranging from photonics to sensing. Most studies have focused on artificial layered materials, while natural layered materials, such as talc and other silicates, have remained largely unexplored despite their desirable properties, e.g., wide direct bandgap, low concentration of optically active defects, and low abundance of nuclear spins. In this article, we carry out a comprehensive computational study of pristine and defective talc layers and discuss their potential applications. After investigating bulk properties, such as lattice parameters, band structure, and dielectric constant, we study the electronic structure, charge states, spin and optical properties of vacancy defects, metal, metalloid, and non-metallic impurities. Our results establish the basis for identifying color centers, electron paramagnetic resonance centers, potential spin quantum bits, and p and n -type dopants. These findings mature the theory of talc and point toward potential applications in quantum technologies.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Electronic and Structural Properties of Oxides · 2D Materials and Applications · Topological Materials and Phenomena
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (50)
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1. Geim, A. K. & Grigorieva, I. V. Van der Waals heterostructures. Nature 499, 419–425 (2013).10.1038/nature12385 ↗
2. Liu, Y. et al. Van der Waals heterostructures and devices. Nat. Rev. Mater. 1, 1–17 (2016).10.1038/natrevmats.2016.42 ↗
3. Liang, S.-J., Cheng, B., Cui, X. & Miao, F. Van der Waals heterostructures for high-performance device applications: challenges and opportunities. Adv. Mater. 32, 1903800 (2020).10.1002/adma.201903800 ↗
4. Healey, A. J. et al. Quantum microscopy with van der Waals heterostructures. Nat. Phys. 1–5 https://www.nature.com/articles/s41567-022-01815-5 (2022).
5. Frisenda, R., Niu, Y., Gant, P., Muñoz, M. & Castellanos-Gomez, A. Naturally occurring van der Waals materials. npj 2D Mater. Appl. 4, 1–13 (2020).10.1038/s41699-020-00172-2 ↗
6. Claverie, M. et al. Synthetic talc and talc-like structures: preparation, features and applications. Chem. Äí A Eur. J. 24, 519–542 (2018).10.1002/chem.201702763 ↗
7. Vasifá, B. et al. Two-dimensional talc as a van der Waals material for solid lubrication at the nanoscale. Nanotechnology 32, 265701 (2021).10.1088/1361-6528/abeffe ↗
8. Mania, E. et al. Spontaneous doping on high quality talc-graphene-hBN van der Waals heterostructures. 2D Mater. 4, 031008 (2017).10.1088/2053-1583/aa76f4 ↗
9. Barcelos, I. D. et al. Infrared fingerprints of natural 2D talc and plasmon, ÄíPhonon coupling in graphene, ÄíTalc heterostructures. ACS Photonics 5, 1912–1918 (2018).10.1021/acsphotonics.7b01017 ↗
10. Gadelha, A. C., Vasconcelos, T. L., Cançado, L. G. & Jorio, A. Nano-optical imaging of in-plane homojunctions in graphene and MoS2 van der Waals heterostructures on talc and SiO2. J. Phys. Chem. Lett. 12, 7625–7631 (2021).10.1021/acs.jpclett.1c01804 ↗
11. Prando, G. A. et al. Revealing excitonic complexes in monolayer WS2 on talc dielectric. Phys. Rev. Appl. 16, 064055 (2021).10.1103/PhysRevApplied.16.064055 ↗
12. Nutting, D. et al. Electrical and optical properties of transition metal dichalcogenides on talc dielectrics. Nanoscale 13, 15853–15858 (2021).10.1039/D1NR04723J ↗
13. Costa, F. J. R., Brito, T. G.-L., Barcelos, I. D. & Zagonel, L. F. Impacts of dielectric screening on the luminescence of monolayer WSe2. Nanotechnology 34, 385703 (2023).10.1088/1361-6528/acda3b ↗
14. Alencar, A. B., Barboza, A. P. M., Archanjo, B. S., Chacham, H. & Neves, B. R. A. Experimental and theoretical investigations of monolayer and few-layer talc. 2D Mater. 2, 015004 (2015).10.1088/2053-1583/2/1/015004 ↗
15. Ma, X., Du, H., Lan, P., Chen, J. & Lan, L. Effect of point defects on electronic properties and structure of talc (001) surface by first principles. Minerals 12, 69 (2022).10.3390/min12010069 ↗
16. Matkovifá, A. et al. Iron-rich talc as air-stable platform for magnetic two-dimensional materials. npj 2D Mater. Appl. 5, 1–9 (2021).10.1038/s41699-020-00190-0 ↗
17. Aharonovich, I., Englund, D. & Toth, M. Solid-state single-photon emitters. Nat. Photonics 10, 631–641 (2016).10.1038/nphoton.2016.186 ↗
18. Awschalom, D. D., Hanson, R., Wrachtrup, J. & Zhou, B. B. Quantum technologies with optically interfaced solid-state spins. Nat. Photonics 12, 516–527 (2018).10.1038/s41566-018-0232-2 ↗
19. Schirhagl, R., Chang, K., Loretz, M. & Degen, C. L. Nitrogen-vacancy centers in diamond: nanoscale sensors for physics and biology. Annu. Rev. Phys. Chem. 65, 83–105 (2014).10.1146/annurev-physchem-040513-103659 ↗
20. Gottscholl, A. et al. Initialization and read-out of intrinsic spin defects in a van der Waals crystal at room temperature. Nat. Mater. 19, 540–545 (2020).10.1038/s41563-020-0619-6 ↗
21. Ivády, V. et al. Ab initio theory of the negatively charged boron vacancy qubit in hexagonal boron nitride. npj Comput. Mater. 6, 1–6 (2020).10.1038/s41524-020-0305-x ↗
22. Stern, H. L. et al. A quantum coherent spin in hexagonal boron nitride at ambient conditions. Nat. Mater. 23, 1379–1385 (2024).10.1038/s41563-024-01887-z ↗
23. Kumar, P. et al. Magnetic imaging with spin defects in hexagonal boron nitride. Phys. Rev. Appl. 18, L061002 (2022).10.1103/PhysRevApplied.18.L061002 ↗
24. Haykal, A. et al. Decoherence of V ${}_{{{{{{{{\rm{b}}}}}}}}}-$ B,àí spin defects in monoisotopic hexagonal boron nitride. Nat. Commun. 13, 4347 (2022).10.1038/s41467-022-31743-0 ↗
25. Tran, T. T., Bray, K., Ford, M. J., Toth, M. & Aharonovich, I. Quantum emission from hexagonal boron nitride monolayers. Nat. Nanotechnol. 11, 37–41 (2016).10.1038/nnano.2015.242 ↗
26. Sajid, A., Ford, M. J. & Reimers, J. R. Single-photon emitters in hexagonal boron nitride: a review of progress. Rep. Prog. Phys. 83, 044501 (2020).10.1088/1361-6633/ab6310 ↗
27. Feres, F. H. et al. Two-dimensional talc as a natural hyperbolic material. Preprint at. https://arxiv.org/abs/2501.17340 (2025).
28. Freysoldt, C. et al. First-principles calculations for point defects in solids. Rev. Mod. Phys. 86, 253–305 (2014).10.1103/RevModPhys.86.253 ↗
29. Zhang, C. et al. Correcting charged supercell defect calculations in low-dimensional semiconductors. Phys. Rev. B 108, 245305 (2023).10.1103/PhysRevB.108.245305 ↗
30. Weston, L., Wickramaratne, D., Mackoit, M., Alkauskas, A. & Van de Walle, C. G. Native point defects and impurities in hexagonal boron nitride. Phys. Rev. B 97, 214104 (2018).10.1103/PhysRevB.97.214104 ↗
31. Thiering, G. & Gali, A. Characterization of oxygen defects in diamond by means of density functional theory calculations. Phys. Rev. B 94, 125202 (2016).10.1103/PhysRevB.94.125202 ↗
32. Benedek, Z., Ganyecz, Á., Pershin, A., Ivády, V. & Barcza, G. Accurate and convergent energetics of color centers by wavefunction theory. https://arxiv.org/abs/2406.05092 (2024).
33. Ivády, V., Abrikosov, I. A., Janzén, E. & Gali, A. Role of screening in the density functional applied to transition-metal defects in semiconductors. Phys. Rev. B 87, 205201 (2013).10.1103/PhysRevB.87.205201 ↗
34. Ivády, V. et al. Theoretical unification of hybrid-DFT and $\text{DFT} + U$ methods for the treatment of localized orbitals. Phys. Rev. B 90, 035146 (2014).10.1103/PhysRevB.90.035146 ↗
35. Tetienne, J.-P. Quantum sensors go flat. Nat. Phys. 17, 1074–1075 (2021).10.1038/s41567-021-01338-5 ↗
36. Kresse, G. & Hafner, J. Ab initio molecular-dynamics simulation of the liquid-metal,Äíamorphous-semiconductor transition in germanium. Phys. Rev. B 49, 14251–14269 (1994).10.1103/PhysRevB.49.14251 ↗
37. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).10.1103/PhysRevB.54.11169 ↗
38. Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).10.1103/PhysRevB.50.17953 ↗
39. Heyd, J., Scuseria, G. E. & Ernzerhof, M. Hybrid functionals based on a screened coulomb potential. J. Chem. Phys. 118, 8207–8215 (2003).10.1063/1.1564060 ↗
40. Heyd, J., Scuseria, G. E. & Ernzerhof, M. Erratum:,"hybrid functionals based on a screened coulomb potential” [j. chem. phys. 118, 8207 (2003)]. J. Chem. Phys. 124, 219906 (2006).10.1063/1.2204597 ↗
41. Henderson, T. M., Paier, J. & Scuseria, G. E. Accurate treatment of solids with the HSE screened hybrid. Phys. Status Solidi (B) 248, 767–774 (2011).10.1002/pssb.201046303 ↗
42. Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J. Chem. Phys. 132, 154104 (2010).10.1063/1.3382344 ↗
43. Gali, A., Janzén, E., Deák, P., Kresse, G. & Kaxiras, E. Theory of spin-conserving excitation of the N-V-$ center in diamond. Phys. Rev. Lett. 103, 186404 (2009).10.1103/PhysRevLett.103.186404 ↗
44. Szász, K., Hornos, T., Marsman, M. & Gali, A. Hyperfine coupling of point defects in semiconductors by hybrid density functional calculations: the role of core spin polarization. Phys. Rev. B 88, 075202 (2013).10.1103/PhysRevB.88.075202 ↗
45. Takács, I. & Ivády, V. Accurate hyperfine tensors for solid state quantum applications: case of the NV center in diamond. Commun. Phys. 7, 178 (2024).10.1038/s42005-024-01668-9 ↗
46. Dancoff, S. M. Non-adiabatic Meson theory of nuclear forces. Phys. Rev. 78, 382–385 (1950).10.1103/PhysRev.78.382 ↗
47. Tamm, I. E., Peierls, R., Bolotovskii, B. M. & Frenkel, V. Y. in Selected Papers, 157–174 (Springer Berlin Heidelberg, 2011). https://books.google.se/books?id=Xg2EMAEACAAJ.
48. Rayner, J. & Brown, G. The crystal structure of talc. Clays Clay Miner. 21, 103–114 (1973).10.1346/CCMN.1973.0210206 ↗
49. Ulian, G., Tosoni, S. & Valdrè, G. Comparison between Gaussian-type orbitals and plane wave ab initio density functional theory modeling of layer silicates: Talc [mg3si4o10 (oh) 2] as model system. J. Chem. Phys. 139, 204101 (2013).10.1063/1.4830405 ↗
50. Robinson, D. A. Measurement of the solid dielectric permittivity of clay minerals and granular samples using a time domain reflectometry immersion method. Vadose Zone J. 3, 705–713 (2004).10.2136/vzj2004.0705 ↗