Excitonic-insulator instability and Peierls distortion in one-dimensional semimetals

in Physical Review. B (2022), 105(7), 075122

The charge density wave instability in one-dimensional semimetals is usually explained through a Peierls-like mechanism, where the coupling of electrons and phonons induces a periodic lattice distortion ... [more ▼]

The charge density wave instability in one-dimensional semimetals is usually explained through a Peierls-like mechanism, where the coupling of electrons and phonons induces a periodic lattice distortion along certain modes of vibration, leading to a gap opening in the electronic band structure and to a lowering of the symmetry of the lattice. In this work, we study two prototypical Peierls systems: the one-dimensional carbon chain and the monatomic hydrogen chain with accurate ab initio calculations based on quantum Monte Carlo and hybrid density functional theory. We demonstrate that in one-dimensional semimetals at T=0, a purely electronic instability can exist independently of a lattice distortion. It is induced by spontaneous formation of low energy electron-hole pairs resulting in the electronic band gap opening, i.e., the destabilization of the semimetallic phase is due to an excitonic mechanism. [less ▲]

Exciton band structure of molybdenum disulfide: from monolayer to bulk

in Electronic Structure (2021), 3

Exciton band structures analysis provides a powerful tool to identify the exciton character of materials, from bulk to isolated systems, and goes beyond the mere analysis of the optical spectra. In this ... [more ▼]

Exciton band structures analysis provides a powerful tool to identify the exciton character of materials, from bulk to isolated systems, and goes beyond the mere analysis of the optical spectra. In this work, we focus on the exciton properties of molybdenum sisulfide (MoS 2 ) by solving the ab initio many-body Bethe–Salpeter equation, as a function of momentum, to obtain the excitation spectra of both monolayer and bulk MoS 2 . We analyse the spectrum and the exciton dispersion on the basis of a model excitonic Hamiltonian capable of providing an efficient description of the excitations in the bulk crystal, starting from the knowledge of the excitons of a single layer. In this way, we obtain a general characterization of both bright and darks excitons in terms of the interplay between the electronic band dispersion (i.e. interlayer hopping) and the electron–hole exchange interaction. We identify for both the 2D and the 3D limiting cases the character of the lowest-energy excitons in MoS 2 , we explain the effects and relative weights of both band dispersion and electron–hole exchange interaction and finally we interpret the differences observed when changing the dimensionality of the system. [less ▲]

Correlation satellites in optical and loss spectra

in Physical Review Research (2020), 2

Coupling of excitations leads to intriguing effects on the spectra of materials. We propose a cumulant formulation for neutral electronic excitations which opens the way to describe effects such as double ... [more ▼]

Coupling of excitations leads to intriguing effects on the spectra of materials. We propose a cumulant formulation for neutral electronic excitations which opens the way to describe effects such as double plasmon satellites or exciton-exciton coupling. Our approach starts from the GW+Bethe-Salpeter approximation to many-body perturbation theory which is based on a quasiparticle picture, and it adds coupling of excitations through a consistent inclusion of dynamically screened interactions. This requires one to consider scattering contributions that are usually neglected. The result is formulated in a way that highlights essential physics, that can be implemented as a postprocessing tool in first-principles codes, and that suggests which kind of materials and measurements should exhibit strong effects. This is illustrated using a model. [less ▲]