The Nature of the Interlayer Interaction in Bulk and Few-Layer Black Phosphorus

Posted on Dec 2, 2015

The Nature of the Interlayer Interaction in Bulk and Few-Layer Black Phosphorus

Phosphorene, a single layer of black phosphorus, is a two dimensional material whose direct semiconducting band-gap, high carrier mobility and sensitivity to strain make it promising for applications. The nature of the binding between layers of black phosphorus was probed using the highly accurate many-body diffusion quantum Monte Carlo approach. A large and unexpected reorganization of electronic charge density was discovered, exposing significant weaknesses in current Density Functional Theory (DFT) approximations.  By identifying the nature of the binding between the layers,  a necessary step has been taken towards understanding the structure and properties of the material.  Identifying a clear failure mode of DFT functionals may guide their future improvement.

For their study of black phosphorus, the research team used the scalable QMCPACK simulation package. With Mira, the Blue Gene Q at ALCF and Sequoia, the Blue Gene Q at Lawrence Livermore National Laboratory, the researchers were able to obtain highly accurate calculations of binding between layers of black phosphorus both in a bilayer and in the bulk.  This demonstrated the accuracy of the method and provided motivation for the calculations of the charge reorganization.

“The Nature of the Interlayer Interaction in Bulk and Few-Layer Phosphorus”, L. Shulenburger, A. D. Baczewski, Z. Zhu, J. Guan, D. Tomanek, Nano Letters, 2015, 10.1021/acs.nanolett.5b03615