Quantum Effects and Phase Tuning in Epitaxial 2H- and 1T -MoTe 2 Monolayers
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1 Supplementary Information Quantum Effects and Phase Tuning in Epitaxial 2H- and 1T -MoTe 2 Monolayers Jinglei Chen, Guanyong Wang,, ǁ Yanan Tang,, Hao Tian,,# Jinpeng Xu, Xianqi Dai,, Hu Xu, # Jinfeng Jia,, ǁ Wingkin Ho, and Maohai Xie,* Physics Department, The University of Hong Kong, Pokfulam Road, Hong Kong Key Laboratory of Artificial Structures and Quantum Control (Ministry of Education), Department of Physics and Astronomy, Shanghai Jiaotong University, 800 Dongchuan Road, Shanghai , China, and ǁ Innovation Center of Advanced Microstructures, Nanjing, China College of Physics and Electronic Engineering, Henan Normal University, Xinxiang, Henan , China, and School of Physics and Electronic Engineering, Zhengzhou Normal University, Zhengzhou, Henan , China # Physics Department, South University of Science and Technology of China, Shenzhen , China. 1
2 KEYWORDS: MoTe 2 monolayer, MBE, STM/STS, quantum effects, phase transition 1 Bandgap determination We follow the method of M. F. Crommie 1 to estimate the energy bandgap of the 2H-phase MoTe 2 ML based on the experimental STS spectrum as shown in Figure 2c (inset) of the main text. The spectrum obtained at 77 K is plotted in logarithm scale. The electronic gap is determined by finding the width of the zero-conductance floor where the band edges are assigned by the intersections of the zero-conductance floor with the linear fits of the conductance data in regions of E VB,2σ E < E < E VB,2σ for the valence band edge and E CB,2σ < E < E CB,2σ + E for the conduction band edge as shown by the red lines in the Figure below. We have chosen ΔE = 50 mv throughout. The complication and uncertainty here arise from the effect of the triangular network of line defects in such films. Because the triangles are relatively small, defects states as well as quantum confinement may affect the measurement, giving rise to non-zero DOS even in the gap region. So there is an uncertainty in determining the zero-conductance floor. Here we have arbitrarily taken it to be the average between -0.7 ev to -0.2 ev, and the estimated bandgap is 1.4 ev, which likely represents an upper bound. 2
3 2. STS measurements over the IDB defects STS measurements at different position of 2H-MoTe 2 are shown in the figure below. The blue curve is the same with Figure 2c of the main text taken in the middle of the triangular domain, which reveals an energy gap. The spectrum taken over the IDB defects (purple), on the other hand, reveals mid-gap states resembling that in epitaxial MoSe 2 as reported earlier Band structure of monolayer 1T MoTe 2 Figure below is the calculated electronic band structure of monolayer 1T -MoTe 2 by density-functional theory, taking account spin-orbit coupling. The optimized lattice constants are a=6.374 Å, b=3.462 Å. The horizontal dashed line marks the energy of the CEC map shown in Fig. 5c in the main text. 3
4 4. Interface of 2H and 1T MoTe 2 Figure below is a STM micrograph (Size: nm 2, sample bias: 2V) showing the interface of the 2H (top) and 1T (bottom) MoTe 2 domains. In the 2H-domain, the contrast is dominated by the IDB defects intertwined into the triangular network. As seen, the interface is quite sharp, which is typical irrespective of their directions. 5. Extracting the RHEED streak intensities To extract the intensities of the RHEED streaks, we firstly take average along the vertical over the selected rectangular box as shown in Figure (a) below and plotted as a function of the horizontal position in Figure (b). Then the two closely spaced satellite peaks corresponding to diffraction from 2H and 1T MoTe 2, respectively, are resolved by multi-peak fittings (green lines in Fig. (b)) and the fitted peak intensities I 1T and I 2H are readout to find the ratio R = I 1T /(I 1T + I 2H ). The data presented in the Fig. 4a of the main text represent averages of three independent measurements and fitting procedures. We have also extracted the areas enclosed by the peaks and calculated the ratios accordingly. The result show very similar trend as in Fig. 4a of the main text, though there is a slight offset in absolute values. 4
5 6. Experiments under different Te fluxes Growth using different Te fluxes but at the same temperature is shown in the figure below, where the growth temperature was constant at 400. It can be seen that the RHEED intensity ratio R, which is related to the domain size of the 1T MoTe 2 increases with Te flux. 7. Annealing with and without Te flux Annealing experiments were also performed, both in vacuum and under the supply of Te flux. The figure presented below summarizes the results at different annealing temperatures while keeping the annealing time fixed at 2 hours. Here, the solid symbols and the black line refer to the data for annealing under vacuum, whereas the open red circles and line are for annealing under the flux of Te. It is seen that increasing annealing temperature leads to a decreasing R (corresponding to an increasing 2H domain or a phase transition from the 1T to 2H phase). On the other hand, the same annealing but under Te flux effectively suppresses such a phase transition. This experiment strongly suggests the important role of surface Te in stabilizing 1T phase MoTe 2. 5
6 8. First principles calculation of Te adsorption on graphene-supported MoTe MoTe 2 laid on top of 6 6 graphene units (see Figs. 2a and 3a in the main text and the Figure below, in which the green balls represent Te atoms, blue balls are Mo while the small black balls are carbon atoms in graphene) were chosen to model Te adsorption effect. Upon adsorbing Te atom(s) on the MoTe 2 surface (e.g., the one circled by the red line in figure below), different adsorption sites were examined by comparing the energies, based on which we determine the most favorable adsorption site to be the hollow site on surface but above the Mo atom by 2.88 Å for 1T and 2.97 Å for 2H cases (refer to figure (a) and (b) below, where the red circles mark the adsorbed Te atom n surface). Having determined the adsorption sites, we then put a varying number of Te atoms (1-8) on the 4 4 MoTe 2 supercell, all on the hollow sites and arranged symmetrically, to model the varying Te coverage from 6.25% (1/4 4) to 50% (8/4 4). In the calculation, except for graphene substrate, all atoms are allowed to relax. Total energy of the system measured relative to a clean (without Te adsorbate) 2H MoTe 2 is plotted in Figure 4b of the main text. 6
7 REFERENCE: 1. Ugeda, M. M.; Bradley, A. J.; Shi, S. F.; da Jornada, F. H.; Zhang, Y.; Qiu, D. Y.; Ruan, W.; Mo, S. K.; Hussain, Z.; Shen, Z. X.; Wang, F.; Louie, S. G.; Crommie, M. F., Giant Bandgap Renormalization and Excitonic Effects in a Monolayer Transition Metal Dichalcogenide Semiconductor. Nat. Mater. 2014, 13, Liu, H.; Jiao, L.; Yang, F.; Cai, Y.; Wu, X.; Ho, W.; Gao, C.; Jia, J.; Wang, N.; Fan, H.; Yao, W.; Xie, M., Dense Network of One-Dimensional Midgap Metallic Modes in Monolayer MoSe2 and Their Spatial Undulations. Phys. Rev. Lett. 2014, 113,
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