TiSe2

A prior report of the emergence of chirality for the (2x2x2) charge density wave (CDW) in TiSe2 has attracted much interest; the drastic symmetry breaking is highly unusual with few precedents [1]. In that study, key evidence was provided by x-ray diffraction measurements of two superlattice reflections, (1.5 1.5 0.5) and (2.5 1 0). The (2.5 1 0) reflection appeared to show an anomalously large intensity and a transition onset at ~7 K below that of the (1.5 1.5 0.5) reflection. These observations, aided by modeling, were cited as evidence for a separate chiral transition. In this Comment, we show that the prior conclusions based on x-ray diffraction are erroneous. There is just one transition, and it is achiral.

Published in: "arXiv Material Science".

The Bose-Einstein condensation of excitons continues to garner immense attention as a prototypical example for observing emergent properties from many-body quantum effects. In particular, Titanium Diselenide (TiSe$_2$) is a promising candidate for realizing exciton condensation and was experimentally observed only very recently [{https://doi.org/10.1126%2Fscience.aam6432}{Science textbf{358} 1314 (2017)}]. Surprisingly, the condensate was experimentally characterized by a soft plasmon mode that only exists near the transition temperature, $T_c$, of the charge density wave (CDW). Here, we characterize and analyze the experimental spectra using linear-response time-dependent density functional theory and find that the soft mode can be attributed to interband electronic transitions. At the CDW state below $T_c$, the periodic lattice distortions hamper the spontaneous formation of the exciton by introducing a CDW gap. Our surprising results contradict previous simplistic analytical models commonly used in the scientific literature. In addition, we find that a finite electronic temperature, $T_e$, introduces an effective band gap and prevents the condensation above $T_c$. The band gap lifts the soft mode and merges it into the regular intraband plasmon. The combined effect of the CDW and $T_e$ explains the fragile temperature-dependence of the exciton condensation. Taken together, our work provides the first textit{ab initio} atomic-level framework for rationalizing recent experiments and further manipulating exciton condensates in TiSe$_2$.

Published in: "arXiv Material Science".

The transition metal dichalcogenide TiSe2 has received signifcant research attention over the past four decades, in large part due to the uniqueness of its charge-ordered state. Different work has presented ways to suppress the charge density wave transition, vary low temperature resistivity by orders of magnitude, and stabilize magnetic or superconducting states. Here we give the results of a new synthesis technique whereby samples were grown in a an argon gas environment at pressures as high as 180 bar. Above 100 K, the properties of these samples are unchanged from previous reports, but a hysteretic resistance region that begins around 80 K accompanied by insulating low temperature behavior are distinct from anything previously observed. This new feature is linked to a decrease in carrier concentration and may allow access to a nonmetallic ground state in a material long speculated to be an excitonic insulator.

Published in: "arXiv Material Science".

The charge density wave (CDW) in 1T-TiSe2 accompanied by the periodic lattice distortion has a nontrivial symmetry configuration. The symmetry is important as an indication of the mechanism and a cue for experimental probes. We examine the symmetry of the system and clear up the connection of electronic structures between the normal and the CDW states. Especially, we unravel the consequential irreducible representations (IRs) of electronic states and, more ahead, those of gap functions among bands when the CDW occurs. Normally symmetry-related topology will be achieved directly, so we assert that the theory is valuable and practical for the search of topological CDW insulators.

Published in: "arXiv Material Science".

We show that the inclusion of screened exchange via hybrid functionals provides a unified description of the electronic and vibrational properties of TiSe2. In contrast to local approximations in density functional theory, the explicit inclusion of exact, non-local exchange captures the effects of the electron-electron interaction needed to both separate the Ti-d states from the Se-p states and stabilize the charge-density-wave (CDW) (or low-T) phase through the formation of a p-d hybridized state. We further show that this leads to an enhanced electron-phonon coupling that can drive the transition even if a small gap opens in the high-T phase. Finally, we demonstrate that the hybrid functionals can generate a CDW phase where the electronic bands, the geometry, and the phonon frequencies are in agreement with experiments.

Published in: "arXiv Material Science".