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Density functional perturbation theory for gated two-dimensional heterostructures: Theoretical developments and application to flexural phonons in graphene

Published 14 May 2017 in cond-mat.mtrl-sci | (1705.04973v2)

Abstract: The ability to perform first-principles calculations of electronic and vibrational properties of two-dimensional heterostructures in a field-effect setup is crucial for the understanding and design of next-generation devices. We present here an implementation of density functional perturbation theories tailored for the case of two-dimensional heterostructures in field-effect configuration. Key ingredients are the inclusion of a truncated Coulomb interaction in the direction perpendicular to the slab and the possibility of simulating charging of the slab via field-effects. With this implementation we can access total energies, force and stress tensors, the vibrational properties and the electron-phonon interaction. We demonstrate the relevance of the method by studying flexural acoustic phonons and their coupling to electrons in graphene doped by field-effect. In particular, we show that while the electron-phonon coupling to those phonons can be significant in neutral graphene, it is strongly screened and negligible in doped graphene, in disagreement with other recent first-principles reports. Consequently, the gate-induced coupling with flexural acoustic modes would not be detectable in transport measurements on doped graphene.

Citations (169)

Summary

Density Functional Perturbation Theory for Gated Two-Dimensional Heterostructures

The paper, authored by Thibault Sohier, Matteo Calandra, and Francesco Mauri, presents substantial advancements in the application of density functional perturbation theory (DFPT) to gated two-dimensional (2D) heterostructures. The study focuses particularly on two-dimensional systems in a field-effect transistor (FET) configuration, offering new insights into their electronic and vibrational properties. This work is pertinent for designing next-generation electronic devices leveraging 2D materials, such as graphene.

Theoretical Developments

The authors address challenges in simulating the properties of 2D materials under experimentally relevant conditions, such as doping induced by electric fields. Traditional density functional theory (DFT) approaches, with three-dimensional periodic boundary conditions, encounter significant limitations when applied to 2D systems. These methods face issues related to spurious interactions from periodic images, especially under long-wavelength perturbations, and cannot adequately simulate the asymmetric field effect present in FET setups.

To overcome these challenges, Sohier et al. implement a density functional perturbation theory specifically tailored for 2D materials. Key to their method is the truncation of Coulomb interactions perpendicular to the slab, effectively isolating each layer. This approach allows for the accurate calculation of total energies, forces, stress tensors, vibrational properties, and electron-phonon interactions in doped 2D systems.

Applications to Flexural Phonons in Graphene

The practical relevance of this theoretical framework is demonstrated through its application to flexural phonons in field-effect doped graphene. Flexural modes, particularly the acoustic out-of-plane (ZA) phonons, are of interest due to their potential impact on electronic properties. The authors significantly contribute by demonstrating the effects of the FET-induced symmetry breaking on the electron-phonon coupling. They report that while a gate-induced electric field can enhance the electron-phonon coupling in neutral graphene, this coupling becomes strongly screened and negligible in doped graphene. This insight is crucial, as it challenges recent first-principles reports and emphasizes the necessity for accurate screening calculations in evaluating the transport properties of doped 2D materials.

Implications and Future Directions

The implications of this research are both theoretical and practical. The newly developed DFPT approach makes it possible to accurately model 2D heterostructures in FET setups, a crucial step for materials science and device engineering. Practically, this means that next-generation electronic devices can be designed with a finer understanding of the underlying material behaviors. Theoretically, the paper enhances our understanding of phonon interactions and electron screening in constrained two-dimensional environments.

Looking ahead, the methods developed in this study pave the way for further exploration of 2D materials in complex configurations, potentially involving various stacking orders and substrate interactions. As the demand for miniaturized and efficient electronic components grows, the need for precise modeling techniques like those presented in this work will undoubtedly increase. Future developments could extend these methodologies to more complex systems, including transition metal dichalcogenides and other van der Waals heterostructures, further broadening the scope of their application in the field of quantum materials and nanotechnology.

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