Gaël Monney

Doping nature of native defects in 1T-TiSe2.

The transition-metal dichalcogenide 1T-TiSe2 is a quasi-two-dimensional layered material with a charge density wave (CDW) transition temperature of T(CDW) ≈ 200 K. Self-doping effects for crystals grown at different temperatures introduce structural defects, modify the temperature-dependent resistivity, and strongly perturbate the CDW phase. Here, we study the structural and doping nature of such native defects combining scanning tunneling microscopy or spectroscopy and ab initio calculations. The dominant native single atom dopants we identify in our single crystals are intercalated Ti atoms, Se vacancies, and Se substitutions by residual iodine and oxygen.

Impact of electron-hole correlations on the 1T-TiSe_{2} electronic structure.

Several experiments have been performed on 1T-TiSe_{2} in order to identify whether the electronic structure is semimetallic or semiconducting without reaching a consensus. In this Letter, we theoretically study the impact of electron-hole and electron-phonon correlations on the bare semimetallic and semiconducting electronic structure. The resulting electron spectral functions provide a direct comparison of both cases and demonstrate that 1T-TiSe_{2} is of predominant semiconducting character with some spectral weight crossing the Fermi level.

Scanning tunneling microscopy of the charge density wave in 1T-TiSe2 in the presence of single atom defects

We present a detailed low-temperature scanning tunneling microscopy (STM) study of the commensurate charge density wave (CDW) in 1T-TiSe2 in the presence of single atom defects. We find no significant modification of the CDW lattice in single crystals with native defect concentrations where some bulk probes already measure substantial reductions in the CDW phase transition signature. A systematic analysis of STM micrographs combined with density functional theory modeling of atomic defect patterns indicate that the observed CDW modulation lies in the Se surface layer. The defect patterns clearly show there are no 2H-polytype inclusions in the CDW phase, as previously found at room temperature [A. N. Titov et al., Phys. Solid State 53, 1073 (2011)]. They further provide an alternative explanation for the chiral Friedel oscillations recently reported in this compound [J. Ishioka et al., Phys. Rev. B 84, 245125 (2011)].

Short-range phase coherence and origin of the 1T-TiSe2 charge density wave

The impact of variable Ti self-doping on the 1T−TiSe2 charge density wave (CDW) is studied by scanning tunneling microscopy. Supported by density functional theory, we show that agglomeration of intercalated-Ti atoms acts as preferential nucleation centers for the CDW that breaks up in phase-shifted CDW domains whose size directly depends on the intercalated-Ti concentration and which are separated by atomically sharp phase boundaries. The close relationship between the diminution of the CDW domain size and the disappearance of the anomalous peak in the temperature-dependent resistivity allows to draw a coherent picture of the 1T−TiSe2 CDW phase transition and its relation to excitons.

Electron?hole instability in 1T-TiSe2

In this paper, we address the question of the origin of the charge density wave instability in 1T-TiSe2. We develop a model considering the direct Coulomb interaction between electrons and holes in the valence and conduction bands near the Fermi energy. Using the Bethe–Salpeter equation, we calculate the electron–hole correlator, which reveals an instability at low temperature leading to a transition toward a commensurate superstructure mediated by the electron–phonon coupling, in agreement with experiments. On the basis of this correlator, the electron self-energies are then calculated and the corresponding photoemission spectra are compared with the experimental ones, revealing good agreement. The signature of electron–hole fluctuations in photoemission is emphasized. Furthermore, we calculate the spectral function of the phonon mode, whose softening is experimentally observed at the transition.

Excited states at interfaces of a metal-supported ultrathin oxide film

We report layer-resolved measurements of the \textit{unoccupied} electronic structure of ultrathin MgO films grown on Ag(001). The metal-induced gap states at the metal/oxide interface, the oxide band gap as well as a surface core exciton involving an image-potential state of the vacuum are revealed through resonant Auger spectroscopy of the Mg

Local resilience of the 1T-TiSe2 charge density wave to Ti self-doping

KL_{23}L_{23}

Selective Probing of Hidden Spin-Polarized States in Inversion-Symmetric Bulk MoS2

Auger transition. Our results demonstrate how to obtain new insights on \textit{empty} states at interfaces of metal-supported ultrathin oxide films.

Mapping of Electron-Hole Excitations in the Charge-Density-Wave System 1T-TiSe2 Using Resonant Inelastic X-Ray Scattering

In Ti-intercalated self-doped 1T-TiSe2 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 long-range phase coherence introduces an imbalance in the intercalated-Ti site distribution and restrains the CDW gap closure. This local resilient behavior of the 1T-TiSe2 CDW reveals an entangled mechanism between CDW, periodic lattice distortion, and induced nonequivalent defects.