Computational methods for 2D materials: discovery, property characterization, and application design.

The discovery of two-dimensional (2D) materials comes at a time when computational methods are mature and can predict novel 2D materials, characterize their properties, and guide the design of 2D materials for applications. This article reviews the recent progress in computational approaches for 2D materials research. We discuss the computational techniques and provide an overview of the ongoing research in the field. We begin with an overview of known 2D materials, common computational methods, and available cyber infrastructures. We then move onto the discovery of novel 2D materials, discussing the stability criteria for 2D materials, computational methods for structure prediction, and interactions of monolayers with electrochemical and gaseous environments. Next, we describe the computational characterization of the 2D materials' electronic, optical, magnetic, and superconducting properties and the response of the properties under applied mechanical strain and electrical fields. From there, we move on to discuss the structure and properties of defects in 2D materials, and describe methods for 2D materials device simulations. We conclude by providing an outlook on the needs and challenges for future developments in the field of computational research for 2D materials.

Pressure-induced superconductivity in the giant Rashba system BiTeI.

At ambient pressure, BiTeI exhibits a giant Rashba splitting of the bulk electronic bands. At low pressures, BiTeI undergoes a transition from trivial insulator to topological insulator. At still higher pressures, two structural transitions are known to occur. We have carried out a series of electrical resistivity and AC magnetic susceptibility measurements on BiTeI at pressure up to ∼40 GPa in an effort to characterize the properties of the high-pressure phases. A previous calculation found that the high-pressure orthorhombic P4/nmm structure BiTeI is a metal. We find that this structure is superconducting with T c values as high as 6 K. AC magnetic susceptibility measurements support the bulk nature of the superconductivity. Using electronic structure and phonon calculations, we compute T c and find that our data is consistent with phonon-mediated superconductivity.

High T_{c} via Spin Fluctuations from Incipient Bands: Application to Monolayers and Intercalates of FeSe.

We investigate superconductivity in a two-band system with an electronlike and a holelike band, where one of the bands is away from the Fermi level (or "incipient"). We argue that the incipient band contributes significantly to spin-fluctuation pairing in the strong coupling limit where the system is close to a magnetic instability and can lead to a large T_{c}. In this case, T_{c} is limited by a competition between the frequency range of the coupling (set by an isolated paramagnon) and the coupling strength itself, such that a domelike T_{c} dependence on the incipient band position is obtained. The coupling of electrons to phonons is found to further enhance T_{c}. The results are discussed in the context of experiments on monolayers and intercalates of FeSe.

First-Principles Calculation of the Real-Space Order Parameter and Condensation Energy Density in Phonon-Mediated Superconductors.

We show that the superconducting order parameter and condensation energy density of phonon-mediated superconductors can be calculated in real space from first principles density functional theory for superconductors. This method highlights the connection between the chemical bonding structure and the superconducting condensation and reveals new and interesting properties of superconducting materials. Understanding this connection is essential to describe nanostructured superconducting systems where the usual reciprocal space analysis hides the basic physical mechanism. In a first application we present results for MgB2, CaC6 and hole-doped graphane.