Combined Scanning Tunneling Microscopy and Noncontact Atomic Force Microscopy Imaging of Silicene Layers on Ag(111) –- Supporting Information –- Andrea Resta1*, Thomas Leoni1, Clemens Barth1, Alain Ranguis1, Conrad Becker1, Thomas Bruhn2, Patrick Vogt2, Guy Le Lay1 1 Aix-Marseille Université, CNRS, CINaM UMR 7325, 13288 Marseille, France. Technische Universität Berlin, Institut für Festkörperphysik, Hardenbergstrasse 36, 10623 Berlin, Germany. 2 Abstract For sake of the article flow some experimental results were not included into the main text. The intent of this supporting information is to round up the information mentioned in the main article. Atomic scale contrasts of STM and nc-AFM images Supp. 1 All the three ncAFM images (a-c) were obtained in the constant mode with the following scanning parameters: Δf = -0.9 Hz ; Ap-p = 4.5 nm, f0 = 26150 Hz, Ubias = -1 V (filled states). The sample was at liquid nitrogen temperature. In the main article we mention typical features in the atomic scale contrast that can be seen in nc-AFM topography images. In Supp. 1 we show three other examples of atomically resolved nc-AFM images with the flower like pattern, which are typical for the silicene 3x3 structure, also regularly found in STM images 1,2,3. Supp. 2: (a) STM topography image (filled states Ubias = -0.8 V, I = 0.4 nA, Ap-p = 10.5 nm), (b) simultaneously recorded current image and (c) Δf image, (d) nc-AFM topography image (Δf=-1.45 Hz, Ap-p = 10.5 nm, Ubias = -0.8 V). (e) Simultaneously recorded current and (f) Δf image. All images were acquired on the sample hold at liquid nitrogen temperature. Image Supp 2(a) is a STM topography image obtained with the Qplus4 sensor oscillating while regulating on the tunneling current. The current set point was at I =0.4 nA, and the current of the current image (Supp 2(b)) ranges from 0.29 nA to 0.39 nA. The detuning image (Supp 2(c)) barely shows any contrast, and to extract the weak contrast here we had to filter part of the noise by averaging over 4 neighbors’ data points. The detuning f ranges from -0.15 Hz to -0.35 Hz. Image Supp 2(d) is a nc-AFM topography image obtained by regulating on the detuning Δf. Image supp. 2(e) contains the current recorded simultaneously while regulating on Δf (range in I: from 0.9 nA to 2 nA). Image Supp. 2(f) contains the Δf signal also recorded together with Supp 2(d) and (e). The detuning ranges between -1 Hz to -3.2 Hz. The images in Supp. 2 support the article’s assumption that the nc-AFM contrast is obtained for tip-surface distances smaller than during STM operation: no atomic contrast in the Δf image in Supp 2(c) can be seen despite the rather high current setting point during the STM operation. Additionally when regulating on Δf = -1.45 Hz and Ubias = 0.8 V in the nc-AFM mode, the current is two to five times larger than the current used to obtain atomic resolution in STM mode at the same bias voltage. As indicated in the main article we report in the insert Figure 2(d) a better contrast on the lower silver terrace (blue region). This region presents the same structure as on the main terrace (red region). A similar situation can also be found in the current image Supp 2(e) where the area corresponding to the lower terrace clearly exhibits the same periodicity as the main terrace. Domains in silicene films Supp. 3 Large scale atomic resolution STM image (Filled states Ubias = 0.4 V, 0.1 nA, Ap-p= 4.5 nm, T = liquid nitrogen temperature). Therein are visible as in figure 4 of the text the two family appearances for the Ag(111)(√13x√13)R± 13.9° superstructure, domains of (3x3) silicene and some islands of the second layer. On the right side LEED patterns from the same surface. The signals frm the Ag(111) substrate are marked in red, the signals from the Ag(111)(√13x√13)R±13.9° are in magenta and those from the Ag(111)(4x4) structure are in green. Supp. 3 contains a large scale STM image with the two families of supercells at ±5.2° and ±33° from the Ag[10] surface vector belonging to the Ag(111)(√13x√13)R±13.9° structure: an hexagonal like moiré pattern and hexagonal array of protrusions. It is also visible that a large part of the surface is covered with a silicene(3x3) structure. Therein are also included a few second layer islands with a silicene(√3x√3)R±30°5,6 structure, which appear as an hexagonal array of protrusion 7. The image here clearly shows the silicene(√3x√3)R±30° as an ad-island. Despite this discrepancy with other works5,6,7, this article confirms and emphasizes the major importance of this phase in the second layer. Here as in the main article we made use of the Wood notation 8 that uses surface unit vectors to describe the supercells. Such vectors are related to the bulk unit vectors: surface Ag[10]= √2/2[1-10]a0, surface Ag[01]= √2/2[0-11] a0 and the vector normal to the surface plane for this new cell become √3[111] a0, were a0 is the bulk lattice constant. In Supp. 3 we also show two Low Energy Electron Diffraction (LEED) patterns. Ag(10) spot of the substrate is marked by the red circle (LEED at 43 eV). magenta circles mark some of the contributions arising from Ag(111)(√13x√13)R±13.9° structure. The green circles mark some of the spots belong to the silicene(3x3) structure. The The the that 1 Vogt, P., De Padova, P., Quaresima, C., Avila, J., Frantzeskakis, E., Asensio, M.C., Resta, A., Ealet, B. & Le Lay, G. Silicene: Compelling Experimental Evidence for Graphenelike TwoDimensional Silicon. Phys. Rev. Lett. 108, 155501 (2012). 2 Lin, C.–L., Arafune, R., Kawahara, K., Tsukahara, N., Minamitani, E., Kim, Y., Takagi, N. & Kawai, M. Structure of Silicene Grown on Ag(111). Appl. Phys. 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