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Register a new userLocal resilience of the $1T$-TiSe$_2$ charge density wave to Ti self-doping
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Added by
Baptiste Hildebrand
Publication date
2016
fields
Physics
and research's language is
English
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In Ti-intercalated self-doped $1T$-TiSe$_2$ crystals, the charge density wave (CDW) superstructure induces two nonequivalent sites for Ti dopants. Recently, it has been shown that increasing Ti doping dramatically influences the CDW by breaking it into phase-shifted domains. Here, we report scanning tunneling microscopy and spectroscopy experiments that reveal a dopant-site dependence of the CDW gap. Supported by density functional theory, we demonstrate that the loss of the longrange phase coherence introduces an imbalance in the intercalated-Ti site distribution and restrains the CDW gap closure. This local resilient behavior of the $1T$-TiSe$_2$ CDW reveals a novel mechanism between CDW and defects in mutual influence.
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In this study, using low-temperature scanning tunneling microscopy (STM), we focus on understanding the native defects in pristine textit{1T}-TiSe$_2$ at the atomic scale. We probe how they perturb the charge density waves (CDWs) and lead to local domain formation. These defects influence the correlation length of CDWs. We establish a connection between suppression of CDWs, Ti intercalation, and show how this supports the exciton condensation model of CDW formation in textit{1T}-TiSe$_2$.
We study the impact of Cu intercalation on the charge density wave (CDW) in 1T-Cu$_{text{x}}$TiSe$_{text{2}}$ by scanning tunneling microscopy and spectroscopy. Cu atoms, identified through density functional theory modeling, are found to intercalate randomly on the octahedral site in the van der Waals gap and to dope delocalized electrons near the Fermi level. While the CDW modulation period does not depend on Cu content, we observe the formation of charge stripe domains at low Cu content (x$<$0.02) and a breaking up of the commensurate order into 2$times$2 domains at higher Cu content. The latter shrink with increasing Cu concentration and tend to be phase-shifted. These findings invalidate a proposed excitonic pairing as the primary CDW formation mechanism in this material.
We investigate the Ti-doping effect on the charge density wave (CDW) of 1T-TaS2 by combining scanning tunneling microscopy (STM) measurements and first-principle calculations. Although the Ti-doping induced phase evolution seems regular with increasing of the doping concentration (x), an unexpected chiral CDW phase is observed in the sample with x = 0.08, in which Ti atoms almost fully occupy the central Ta atoms in the CDW clusters. The emergence of the chiral CDW is proposed to be from the doping-enhanced orbital order. Only when x = 0.08, the possible long-range orbital order can trigger the chiral CDW phase. Compared with other 3d-elements doped 1T-TaS2, the Ti-doping retains the electronic flat band and the corresponding CDW phase, which is a prerequisite for the emergence of chirality. We expect that introducing elements with a strong orbital character may induce a chiral charge order in a broad class of CDW systems. The present results open up another avenue for further exploring the chiral CDW materials.
We report temperature-dependent transport and x-ray diffraction measurements of the influence of Ti hole doping on the charge density wave (CDW) in 1T-Ta(1-x)Ti(x)S(2). Confirming past studies, we find that even trace impurities eliminate the low-temperature commensurate (C) phase in this system. Surprisingly, the magnitude of the in-plane component of the CDW wave vector in the nearly commensurate (NC) phase does not change significantly with Ti concentration, as might be expected from a changing Fermi surface volume. Instead, the angle of the CDW in the basal plane rotates, from 11.9 deg at x=0 to 16.4 deg at x=0.12. Ti substitution also leads to an extended region of coexistence between incommensurate (IC) and NC phases, indicating heterogeneous nucleation near the transition. Finally, we explain a resistive anomaly originally observed by DiSalvo [F. J. DiSalvo, et al., Phys. Rev. B {bf 12}, 2220 (1975)] as arising from pinning of the CDW on the crystal lattice. Our study highlights the importance of commensuration effects in the NC phase, particularly at x ~ 0.08.
A variety of experiments have been carried out to establish the origin of the chiral charge-density wave transition in 1T-TiSe$_2$, which in turn has led to contradictory conclusions on the origin of this transition. Some studies suggest the transition is a phonon-driven structural distortion while other studies suggest it is an excitonic insulator phase transition that is accompanied by a lattice distortion. First, we propose these interpretations can be reconciled if one analyzes the available experimental and theoretical data within a formal definition of what constitutes an excitonic insulator as initially proposed by Keldysh and Kopaev. Next, we present pump-probe measurements of circularly polarized optical transitions and first-principles calculations where we highlight the importance of accounting for structural distortions to explain the finite chirality of optical transitions in the CDW phase. We show that at the elevated electronic temperature that occurs upon photoexcitation, there is a non-centrosymmetric structure that is near-degenerate in energy with the centrosymmetric charge density wave structure, which explains the finite chirality of the optical transitions observed in the CDW phase of TiSe$_2$.
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