Excitonic effects in two-dimensional TiSe${}_2$ from hybrid density functional theory

Abstract

Transition metal dichalcogenides (TMDs), whether in bulk or in monolayer form, exhibit a rich variety of charge-density-wave (CDW) phases and stronger periodic lattice distortions. While the actual role of nesting has been under debate, it is well understood that the microscopic interaction responsible for the CDWs is the electron-phonon coupling. The case of TiSe${}_2$ is however unique in this family in that the normal state above the critical temperature $T_{\mathrm{CDW}}$ is characterized by a small quasiparticle bandgap as measured by ARPES, so that no nesting-derived enhancement of the susceptibility is present. It has therefore been argued that the mechanism responsible for this CDW should be different and that this material realizes the excitonic insulator phase proposed by Walter Kohn. On the other hand, it has also been suggested that the whole phase diagram can be explained by a sufficiently strong electron-phonon coupling. In this work, in order to estimate how close this material is to the pure excitonic insulator instability, we quantify the strength of electron-hole interactions by computing the exciton band structure at the level of hybrid density functional theory, focusing on the monolayer. We find that in a certain range of parameters the indirect gap at $q_{\mathrm{CDW}}$ is significantly reduced by excitonic effects. We discuss the consequences of those results regarding the debate on the physical mechanism responsible for this CDW. Based on the dependence of the calculated exciton binding energies as a function of the mixing parameter of hybrid DFT, we conjecture that a necessary condition for a pure excitonic insulator is that its noninteracting electronic structure is metallic.

arXiv comment6 pages, 3 figures

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Cited by in corpus (8)

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• Heterobilayers of 2D materials as a platform for excitonic superfluidity
• Ab initio phonon self-energies and fluctuation diagnostics of phonon anomalies: Lattice instabilities from Dirac pseudospin physics in transition metal dichalcogenides
• Charge Density Wave Hampers Exciton Condensation in 1T-TiSe${}_2$
• Electronic structure of TiSe${}_2$ from a quasi-self-consistent G${}_0$W${}_0$ approach
• Impact ionization dynamics in small band-gap 2D materials from a coherent phonon mechanism
• Optical amplification in a CDW-phase of a quasi-two dimensional material
• Excitons and Optical Response in Excitonic Insulator Candidate TiSe${}_2$