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Tersoff, J.; Hamann, D. R. Theory and application for the scanning tunneling microscope. Phys. Rev. Lett. 1983, 50, 1998–2001. Li, F. P.; Wei, W.; Lv, X. S.; Huang, B. B.; Dai, Y. Evolution of the linear band dispersion of monolayer and bilayer germanene on Cu(111). Phys. Chem. Chem. Phys. 2017, 19, 22844–22851. Cahangirov, S.; Topsakal, M.; Aktürk, E.; Şahin, H.; Ciraci, S. Two- and one-dimensional honeycomb structures of silicon and germanium. Phys. Rev. Lett. 2009, 102, 236804. The growth fronts of the (√67 × √67)R12.2° double layer oxide phase shown in Fig. 2 do not proceed along straight but rather kinked edges indicating the rotational misalignment of the surface oxide and the underlying substrate. The image sequence of Fig. 2 (movie in ESI-b †) proves that this growth mode along kinked edges results in a seemingly random outward growth of the double layer oxide from the former step edges together with an inward growth on the terrace until finally the whole terrace is covered by the oxide phase. Thus, dosing O 2 to the Ni 3Al(111) surface at temperatures more than 60 K above the formation temperature of the (7 × 7) single layer oxide (740 K) leads to the growth of the (√67 × √67)R12.2° double layer oxide. J. A. Kelber, Alumina surfaces and interfaces under non-ultrahigh vacuum conditions, Surf. Sci. Rep., 2007, 62(7), 271–303 CrossRef CAS.

Chaika, A. N.; Orlova, N. N.; Semenov, V. N.; Postnova, E. Y.; Krasnikov, S. A.; Lazarev, M. G.; Chekmazov, S. V.; Aristov, V. Y.; Glebovsky, V. G.; Bozhko, S. I.; et al. Fabrication of [001]-oriented tungsten tips for high resolution scanning tunneling microscopy. Sci Rep 2014, 4, 3742. Derivaz, M.; Dentel, D.; Stephan, R.; Hanf, M. C; Mehdaoui, A.; Sonnet, P.; Pirri, C. Continuous germanene layer on Al(111). Nano Lett. 2015, 15, 2510–2516.Muzychenko, D. A.; Oreshkin, A. I.; Oreshkin, S. I.; Ustavschikov, S. S.; Putilov, A. V.; Aladyshkin, A. Y. The surface structures growth’s features caused by Ge adsorption on the Au(111) surface. JETP Lett. 2017, 106, 217–222. W. G. Moffat, The handbook of binary phase diagrams, Genium Publishing Corp, New York, 1976 Search PubMed.

E. W. A. Young, J. C. Rivière and L. S. Welch, Investigation by X-ray photoelectron spectroscopy of the transient oxidation of NiAl, Appl. Surf. Sci., 1987, 28(1), 71–84 CrossRef CAS.

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Gou, J.; Kong, L. J.; Li, H.; Zhong, Q.; Li, W. B.; Cheng, P.; Chen, L.; Wu, K. H. Strain-induced band engineering in monolayer stanene on Sb(111). Phys. Rev. Mater. 2017, 1, 054004. M. Schmid, G. Kresse, A. Buchsbaum, E. Napetschnig, S. Gritschneder, M. Reichling and P. Varga, Nanotemplate with Holes: Ultrathin Alumina on Ni 3Al(111), Phys. Rev. Lett., 2007, 99(19), 196104 CrossRef CAS PubMed. Herz, M.; Giessibl, F. J.; Mannhart, J. Probing the shape of atoms in real space. Phys. Rev. B 2003, 68, 045301. Lin, C. H.; Huang, A.; Pai, W. W.; Chen, W. C.; Chang, T. R.; Yukawa, R.; Cheng, C. M.; Mou, C. Y.; Matsuda, I.; Chiang, T. C. et al. Single-layer dual germanene phases on Ag(111). Phys. Rev. Mater. 2018, 2, 024003. Rohlfing, M.; Temirov, R.; Tautz, F. S. Adsorption structure and scanning tunneling data of a prototype organic-inorganic interface: PTCDA on Ag(111). Phys. Rev. B 2007, 76, 115421.

Horcas, I.; Fernández, R.; Gómez-Rodríguez, J. M.; Colchero, J.; Gómez-Herrero, J.; Baro, A. M. WSXM: A software for scanning probe microscopy and a tool for nanotechnology. Rev. Sci. Instrum. 2007, 78, 013705.When lowering the temperature during O 2 exposure by about 20–30 K below the growth temperature of the (7 × 7) single layer aluminum oxide phase, a novel bilayer surface oxide phase is formed. This indicates that also the low temperature double layer surface oxide must be a metastable phase with a slightly lower formation energy per oxygen atom than the (7 × 7) single layer oxide phase. However, since lowering the substrate temperature leads to the formation of the novel bilayer oxide instead of the single layer oxide, an effective energy barrier E B1 smaller than the one to be overcome for the formation of the (7 × 7) phase has to exist. Again, once built, the bilayer oxide does not transform into the (7 × 7) single layer oxide phase during growth, because the energy required ( E X1& E B2) exceeds E B1, why the surface may be entirely covered by the low temperature bilayer oxide phase.

A. Arranz and C. Palacio, Interaction of Ni/Al Interfaces with Oxygen, Langmuir, 2002, 18(5), 1695–1701 CrossRef CAS. The growth of the different oxide phases is controlled not only by the deficiency of Al but also by the excess of metal atoms that have to be laterally displaced on the surface. The Al coverage of the (7 × 7) single layer oxide was shown to amount about 0.5 ML. 44 Thus, during formation of the single layer oxide 0.5 ML excess metal atoms are formed that were shown to diffuse on the terrace until they reach the ascending step edge where the single layer oxide phase is also formed. At lower temperature the time required to build the single layer phase might exceed the one of generating diffusing metal adatoms or diffusing metal–oxygen units on the surface. As a result, the concentration of such diffusing species would increase with time. If the species were trapped on top of the already built single oxide phase, naturally the 2nd layer phase will be formed due to the unbalancing of the generation and consumption rate of metal atoms on the Ni 3Al(111) surface. C.-Y. Ho, R. B. Patil, C.-C. Wang, C.-S. Chao, Y.-D. Li, H.-C. Hsu, M.-F. Luo, Y.-C. Lin, Y.-L. Lai and Y.-J. Hsu, Methanol-driven structuring of Au–Pt bimetallic nanoclusters on a thin film of Al 2O 3/NiAl(100), Surf. Sci., 2012, 606(15), 1173–1179 CrossRef CAS. A. M. Venezia and C. M. Loxton, Low pressure oxidation of Ni 3Al alloys at elevated temperatures as studied by X-ray photoelectron spectroscopy and Auger spectroscopy, Surf. Sci., 1988, 194(1), 136–148 CrossRef CAS. Qin, Z. H.; Pan, J. B.; Lu, S. Z.; Shao, Y.; Wang, Y. L.; Du, S. X.; Gao, H. J.; Cao, G. Y. Direct evidence of dirac signature in bilayer germanene islands on Cu(111). Adv. Mater. 2017, 29, 1606046.

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We have obtained single phase monolayer germanene on aluminum (111) thin films grown on a germanium (111) template by atomic segregation epitaxy, a preparation method differing from molecular beam epitaxy used in previous works. This 2 × 2 reconstructed germanene phase matching an Al(111)3 × 3 supercell has been prepared in large areas upon annealing at 430 °C. Detailed studies have been carried out using scanning tunneling microscopy (STM), low-energy electron diffraction, Auger electron spectroscopy, and synchrotron radiation photoemission spectroscopy. First-principles calculations based on the density function theory along with atomic-scale STM images reveal the atomic structure with one protruding Ge atom per 2 × 2 germanene supercell and a characteristic dispersing band originating from the germanene sheet slightly coupled to the first layer Al atoms underneath. Instead, upon annealing at lower temperatures, multi-phase regions comprise twisted germanene domains in correspondence with an Al(111)√7 ×√7 R ± 19.1° superstructure as obtained in previous studies. Perdew, J. P.; Burke, K.; Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 1996, 77, 3865–3868.

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