- Zhang, Yi;
- Ugeda, Miguel M;
- Jin, Chenhao;
- Shi, Su-Fei;
- Bradley, Aaron J;
- Martín-Recio, Ana;
- Ryu, Hyejin;
- Kim, Jonghwan;
- Tang, Shujie;
- Kim, Yeongkwan;
- Zhou, Bo;
- Hwang, Choongyu;
- Chen, Yulin;
- Wang, Feng;
- Crommie, Michael F;
- Hussain, Zahid;
- Shen, Zhi-Xun;
- Mo, Sung-Kwan
High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct-indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.