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F. Vanini

Publications and source records attributed to F. Vanini.

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Unveiling the Semimetallic Nature of 1$T$-TiSe$_2$ by Doping its Charge Density Wave

The semimetallic or semiconducting nature of the transition metal dichalcogenide 1$T$-TiSe$_2$ remains under debate after many decades mainly due to the fluctuating nature of its 2 $\times$ 2 $\times$ 2 charge-density-wave (CDW) phase at room-temperature. In this letter, using angle-resolved photoemission spectroscopy, we unambiguously demonstrate that the 1$T$-TiSe$_2$ normal state is semimetallic with an electron-hole band overlap of $\sim$110 meV by probing the low-energy electronic states of the perturbed CDW phase strongly doped by alkali atoms. Our study not only closes a long-standing debate but also supports the central role of the Fermi surface for driving the CDW and superconducting instabilities in 1$T$-TiSe$_2$.

cond-mat.str-el

Semimetal-to-semiconductor transition and charge-density-wave melting in $1T$-TiSe$_{2-x}$S$_x$ single crystals

The transition metal dichalcogenide $1T$-TiSe$_2$ is a quasi-two-dimensional layered material with a phase transition towards a commensurate charge density wave (CDW) at a critical temperature T$_{c}\approx 200$K. The relationship between the origin of the CDW instability and the semimetallic or semiconducting character of the normal state, i.e., with the non-reconstructed Fermi surface topology, remains elusive. By combining angle-resolved photoemission spectroscopy (ARPES), scanning tunneling microscopy (STM), and density functional theory (DFT) calculations, we investigate $1T$-TiSe$_{2-x}$S$_x$ single crystals. Using STM, we first show that the long-range phase coherent CDW state is stable against S substitutions with concentrations at least up to $x=0.34$. The ARPES measurements then reveal a slow but continuous decrease of the overlap between the electron and hole ($e$-$h$) bands of the semimetallic normal-state well reproduced by DFT and related to slight reductions of both the CDW order parameter and $T_c$. Our DFT calculations further predict a semimetal-to-semiconductor transition of the normal state at a higher critical S concentration of $x_c$=0.9 $\pm$0.1, that coincides with a melted CDW state in TiSeS as measured with STM. Finally, we rationalize the $x$-dependence of the $e$-$h$ band overlap in terms of isovalent substitution-induced competing chemical pressure and charge localization effects. Our study highlights the key role of the $e$-$h$ band overlap for the CDW instability.

cond-mat.mtrl-sci

Phase Separation in the Vicinity of Fermi Surface Hot Spots

Spatially inhomogeneous electronic states are expected to be key ingredients for the emergence of superconducting phases in quantum materials hosting charge-density-waves (CDWs). Prototypical materials are transition-metal dichalcogenides (TMDCs) and among them, 1$T$-TiSe$_2$ exhibiting intertwined CDW and superconducting states under Cu intercalation, pressure or electrical gating. Although it has been recently proposed that the emergence of superconductivity relates to CDW fluctuations and the development of spatial inhomogeneities in the CDW order, the fundamental mechanism underlying such a phase separation (PS) is still missing. Using angle-resolved photoemission spectroscopy and variable-temperature scanning tunneling microscopy, we report on the phase diagram of the CDW in 1$T$-TiSe$_2$ as a function of Ti self-doping, an overlooked degree of freedom inducing CDW texturing. We find an intrinsic tendency towards electronic PS in the vicinity of Fermi surface (FS) "hot spots", i.e. locations with band crossings close to, but not at the Fermi level. We therefore demonstrate an intimate relationship between the FS topology and the emergence of spatially textured electronic phases which is expected to be generalizable to many doped CDW compounds.

cond-mat.mtrl-sci

Local resilience of the $1T$-TiSe$_2$ charge density wave to Ti self-doping

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.

cond-mat.mtrl-sci

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 $KL_{23}L_{23}$ Auger transition. Our results demonstrate how to obtain new insights on \textit{empty} states at interfaces of metal-supported ultrathin oxide films.

cond-mat.mtrl-sci