Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Letter
  • Open Access

Role of doping in probe microscopies for the Si(111) 7×7 surface

Dingxin Fan

Yuki Sakai

James R. Chelikowsky

Daniel Meuer

Alfred J. Weymouth

Franz J. Giessibl

  • Department of Physics, McKetta Department of Chemical Engineering, Center for Computational Materials, Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, USA

Phys. Rev. Research 7, L012046 – Published 27 February, 2025

DOI: https://doi.org/10.1103/PhysRevResearch.7.L012046

Abstract

We investigate a scanning probe microscopy image flickering phenomenon, i.e., distinct changes in intensity with the tip height, observed on a B-doped Si(111) 7×7 reconstructed surface. The phenomenon is exclusively observed in heavily doped systems owing to large variations in the adatom heights (∼0.5 a.u.) and the existence of bistable subunits upon doping as the probe tip approaches the surface. We find that B atoms prefer to reside in the surface layer, which is ∼1.1 eV more stable compared to interior layers. These dopant atoms exert a substantial influence on the structural integrity and electronic structure of the lattice.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (52)

  1. J. Chelikowsky, Why silicon is the benchmark, Mater. Today 5, 64 (2002).
  2. R. E. Schlier and H. E. Farnsworth, Structure and adsorption characteristics of clean surfaces of germanium and silicon, J. Chem. Phys. 30, 917 (1959).
  3. J. E. Demuth, B. N. J. Persson, and A. J. Schell-Sorokin, Temperature-dependent surface states and transitions of Si(111)-7×7, Phys. Rev. Lett. 51, 2214 (1983).
  4. F. J. Giessibl, Atomic resolution of the silicon (111)-(7×7) surface by atomic force microscopy, Science 267, 68 (1995).
  5. M. Emmrich et al., Subatomic resolution force microscopy reveals internal structure and adsorption sites of small iron clusters, Science 348, 308 (2015).
  6. Y. Hasegawa, I.-W. Lyo, and P. Avouris, Measurement of surface state conductance using STM point contacts, Surf. Sci. 357–358, 32 (1996).
  7. K. Yoo and H. H. Weitering, Electrical conductance of reconstructed silicon surfaces, Phys. Rev. B 65, 115424 (2002).
  8. M. A. Lantz, H. J. Hug, R. Hoffmann, S. Martin, A. Baratoff, and H. J. Güntherodt, Short-range electrostatic interactions in atomic-resolution scanning force microscopy on the Si(111)7×7 surface, Phys. Rev. B 68, 035324 (2003).
  9. T. Eguchi and Y. Hasegawa, High resolution atomic force microscopic imaging of the Si(111)-(7×7) surface: Contribution of short-range force to the images, Phys. Rev. Lett. 89, 266105 (2002).
  10. T. L. Chan, C. Z. Wang, K. M. Ho, and J. R. Chelikowsky, Efficient first-principles simulation of noncontact atomic force microscopy for structural analysis, Phys. Rev. Lett. 102, 176101 (2009).
  11. S. H. Ke, T. Uda, and K. Terakura, Surface topography of the Si(111)7×7 reconstruction, Phys. Rev. B 62, 15319 (2000).
  12. M. Smeu, H. Guo, W. Ji, and R. A. Wolkow, Electronic properties of Si(111)-7×7 and related reconstructions: Density functional theory calculations, Phys. Rev. B 85, 195315 (2012).
  13. K. Takayanagi, Y. Tanishiro, M. Takahashi, and S. Takahashi, Structural analysis of Si(111)-7×7 by UHV-transmission electron diffraction and microscopy, J. Vac. Sci. Technol. A 3, 1502 (1985).
  14. G. Binnig, H. Rohrer, C. Gerber, and E. Weibel, 7×7 reconstruction on Si(111) resolved in real space, Phys. Rev. Lett. 50, 120 (1983).
  15. F. J. Giessibl, H. Bielefeldt, S. Hembacher, and J. Mannhart, Imaging of atomic orbitals with the Atomic Force Microscope—experiments and simulations, Ann. Phys. 513, 887 (2001).
  16. D. Fan, Y. Sakai, and J. R. Chelikowsky, Real-space pseudopotential calculations for simulating noncontact atomic force microscopy images, J. Vac. Sci. Technol. B 36, 04H102 (2018).
  17. M. Kim and J. R. Chelikowsky, CO tip functionalization in subatomic resolution atomic force microscopy, Appl. Phys. Lett. 107, 163109 (2015).
  18. A. J. Lee, Y. Sakai, M. Kim, and J. R. Chelikowsky, Repulsive tip tilting as the dominant mechanism for hydrogen bond-like features in atomic force microscopy imaging, Appl. Phys. Lett. 108, 193102 (2016).
  19. L. Gross, F. Mohn, N. Moll, P. Liljeroth, and G. Meyer, The chemical structure of a molecule resolved by atomic force microscopy, Science 325, 1110 (2009).
  20. L. Gross, F. Mohn, N. Moll, B. Schuler, A. Criado, E. Guitián, D. Peña, A. Gourdon, and G. Meyer, Bond-order discrimination by atomic force microscopy, Science 337, 1326 (2012).
  21. D. G. de Oteyza et al., Direct imaging of covalent bond structure in single-molecule chemical reactions, Science 340, 1434 (2013).
  22. J. Zhang, P. Chen, B. Yuan, W. Ji, Z. Cheng, and X. Qiu, Real-space identification of intermolecular bonding with atomic force microscopy, Science 342, 611 (2013).
  23. A. Riss et al., Local electronic and chemical structure of oligo-acetylene derivatives formed through radical cyclizations at a surface, Nano Lett. 14, 2251 (2014).
  24. M. P. Boneschanscher, J. van der Lit, Z. Sun, I. Swart, P. Liljeroth, and D. Vanmaekelbergh, Quantitative atomic resolution force imaging on epitaxial graphene with reactive and nonreactive AFM probes, ACS Nano 6, 10216 (2012).
  25. M. Ellner, N. Pavliček, P. Pou, B. Schuler, N. Moll, G. Meyer, L. Gross, and R. Peréz, The electric field of CO tips and its relevance for atomic force microscopy, Nano Lett. 16, 1974 (2016).
  26. P. Jelínek, High resolution SPM imaging of organic molecules with functionalized tips, J. Phys.: Condens. Matter 29, 343002 (2017).
  27. S. Kawai, T. Nishiuchi, T. Kodama, P. Spijker, R. Pawlak, T. Meier, J. Tracey, T. Kubo, E. Meyer, and A. S. Foster, Direct quantitative measurement of the C═O⋅⋅⋅H–C bond by atomic force microscopy, Sci. Adv. 3, e1603258 (2017).
  28. D. Fan and J. R. Chelikowsky, Atomic fingerprinting of heteroatoms using noncontact atomic force microscopy, Small 17, 2102977 (2021).
  29. P. Chen, D. Fan, A. Selloni, E. A. Carter, C. B. Arnold, Y. Zhang, A. S. Gross, J. R. Chelikowsky, and N. Yao, Observation of electron orbital signatures of single atoms within metal-phthalocyanines using atomic force microscopy, Nat. Commun. 14, 1460 (2023).
  30. D. Fan, Y. Sakai, and J. R. Chelikowsky, Chemical and steric effects in simulating noncontact atomic force microscopy images of organic molecules on a Cu (111) substrate, Phys. Rev. Mater. 4, 053802 (2020).
  31. D. Fan, Y. Sakai, and J. R. Chelikowsky, Discrimination of bond order in organic molecules using noncontact atomic force microscopy, Nano Lett. 19, 5562 (2019).
  32. P. Chen, D. Fan, Y. Zhang, A. Selloni, E. A. Carter, C. B. Arnold, D. C. Dankworth, S. P. Rucker, J. R. Chelikowsky, and N. Yao, Breaking a dative bond with mechanical forces, Nat. Commun. 12, 5635 (2021).
  33. T. R. Albrecht, P. Grütter, D. Horne, and D. Rugar, Frequency modulation detection using high-Q cantilevers for enhanced force microscope sensitivity, J. Appl. Phys. 69, 668 (1991).
  34. A. Peronio, N. Okabayashi, F. Griesbeck, and F. Giessibl, Radio frequency filter for an enhanced resolution of inelastic electron tunneling spectroscopy in a combined scanning tunneling- and atomic force microscope, Rev. Sci. Instrum. 90, 123104 (2019).
  35. F. J. Giessibl, Forces and frequency shifts in atomic-resolution dynamic-force microscopy, Phys. Rev. B 56, 16010 (1997).
  36. P. Hohenberg and W. Kohn, Inhomogeneous electron gas, Phys. Rev. 136, B864 (1964).
  37. W. Kohn and L. J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140, A1133 (1965).
  38. See Supplemental Material at http://link.aps.org/supplemental/10.1103/PhysRevResearch.7.L012046 for computational details and experimental movie clips.
  39. X. Huang, E. Lindgren, and J. R. Chelikowsky, Surface passivation method for semiconductor nanostructures, Phys. Rev. B 71, 165328 (2005).
  40. S. Öğüt, J. R. Chelikowsky, and S. G. Louie, Quantum confinement and optical gaps in Si nanocrystals, Phys. Rev. Lett. 79, 1770 (1997).
  41. T.-L. Chan, H. Kwak, J.-H. Eom, S. B. Zhang, and J. R. Chelikowsky, Self-purification in Si nanocrystals: An energetics study, Phys. Rev. B 82, 115421 (2010).
  42. H. Huang, S. Y. Tong, W. E. Packard, and M. B. Webb, Atomic geometry of Si(111) 7×7 by dynamical low-energy electron diffraction, Phys. Lett. A 130, 166 (1988).
  43. S. Y. Tong, H. Huang, C. M. Wei, W. E. Packard, F. K. Men, G. Glander, and M. B. Webb, Low-energy electron diffraction analysis of the Si(111)7×7 structure, J. Vac. Sci. Technol. A 6, 615 (1988).
  44. T. Uchihashi, Y. Sugawara, T. Tsukamoto, M. Ohta, S. Morita, and M. Suzuki, Role of a covalent bonding interaction in noncontact-mode atomic-force microscopy on Si(111)7×7, Phys. Rev. B 56, 9834 (1997).
  45. D. Eom, C.-Y. Moon, and J.-Y. Koo, Switching the charge state of individual surface atoms at Si(111)-√3×√3:B surfaces, Nano Lett. 15, 398 (2015).
  46. L. Kronik, A. Makmal, M. L. Tiago, M. M. G. Alemany, M. Jain, X. Huang, Y. Saad, and J. R. Chelikowsky, PARSEC–the pseudopotential algorithm for real-space electronic structure calculations: Recent advances and novel applications to nano-structures, Phys. Status Solidi B 243, 1063 (2006).
  47. J. R. Chelikowsky, N. Troullier, and Y. Saad, Finite-difference-pseudopotential method: Electronic structure calculations without a basis, Phys. Rev. Lett. 72, 1240 (1994).
  48. R. C. James, The pseudopotential-density functional method applied to nanostructures, J. Phys. D: Appl. Phys. 33, R33 (2000).
  49. J. R. Chelikowsky, N. Troullier, K. Wu, and Y. Saad, Higher-order finite-difference pseudopotential method: An application to diatomic molecules, Phys. Rev. B 50, 11355 (1994).
  50. A. Natan, A. Benjamini, D. Naveh, L. Kronik, M. L. Tiago, S. P. Beckman, and J. R. Chelikowsky, Real-space pseudopotential method for first principles calculations of general periodic and partially periodic systems, Phys. Rev. B 78, 075109 (2008).
  51. Z. Sun, M. P. Boneschanscher, I. Swart, D. Vanmaekelbergh, and P. Liljeroth, Quantitative atomic force microscopy with carbon monoxide terminated tips, Phys. Rev. Lett. 106, 046104 (2011).
  52. D. J. Chadi and K. J. Chang, Energetics of DX-center formation in GaAs and AlxGa1−xAs alloys, Phys. Rev. B 39, 10063 (1989).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation