Jae-Hyeok Ko1,Woosun Jang2,Aloysius Soon1
Yonsei University1,Seoul National University2
Jae-Hyeok Ko1,Woosun Jang2,Aloysius Soon1
Yonsei University1,Seoul National University2
Heterointerfaces of two-dimensional (2D) van der Waals (vdW) nanomaterials often exhibit unusual, “<i>non-textbook</i>” bonding mechanism that involves distinct (i.e., weak but non-negligible) orbital coupling within the compressed vdW gap [1]. This unique bonding mechanism is speculated to be quite different from the previously reported charge compression effect in ultrathin oxide films on metals [2]. To unravel this atypical bonding mechanism for 2D heterointerfaces, using vdW-corrected density-functional theory calculations, we examine the compressed charge redistribution in the heterostructures of ReSe<sub>2</sub>/graphene and ReSe<sub>2</sub>/h-BN. Here, we report the optimized atomic structures, electronic density-of-states, (integrated) planar-averaged electron density differences for these heterostructures, while focusing on the explicit contributions of the conductive graphene and insulating h-BN substrates to the interlayer confined charges. We demonstrate that this charge compression effect in the vdW gap is ubiquitous regardless of the nature of the substrates, and the magnitude of the confined charges can be modulated by atomic strain engineering. This study highlights the importance of understanding the interlayer charge compression effects by tailoring work function design for low-dimensional device applications [3].<br/><br/>[1] T. T. Ly, Y.-J. Lee, B. K. Choi, H. Lee, H. J. Kim, G. Duvjir, N. H. Lam, K. Jang, K. Palotás, Y. J. Chang, A. Soon, and J. Kim, <i>Appl. Surf. Sci.</i> <b>579</b>, 152187 (2022).<br/>[2] L. Giordano, F. Cinquini, and G. Pacchioni, <i>Phys. Rev. B.</i> <b>73</b>, 045414 (2006).<br/>[3] W. Jang, J. Lee, C. In, H. Choi, and A. Soon, <i>ACS Appl. Mater. Interfaces</i> <b>9</b>, 42050 (2017).