Abstract
The dosing of layered materials with alkali metals has become a commonly used strategy in ARPES experiments. However, precisely what occurs under such conditions, both structurally and electronically, has remained a matter of debate. Here we perform a systematic study of 1T-${\mathrm{HfTe}}_{2}$, a prototypical semimetal of the transition metal dichalcogenide family. By utilizing photon energy-dependent angle-resolved photoemission spectroscopy (ARPES), we have investigated the electronic structure of this material as a function of potassium (K) deposition. From the ${k}_{z}$ maps, we observe the appearance of 2D dispersive bands after electron dosing, with an increasing sharpness of the bands, consistent with the wave-function confinement at the topmost layer. In our highest-dosing cases, a monolayerlike electronic structure emerges, presumably as a result of intercalation of the alkali metal. Here, by bringing the topmost valence band below ${E}_{F}$, we can directly measure a band overlap of $\ensuremath{\sim}0.2$ eV. However, 3D bulklike states still contribute to the spectra even after considerable dosing. Our work provides a reference point for the increasingly popular studies of the alkali metal dosing of semimetals using ARPES.
Highlights
Alkali metal deposition on layered materials has turned into a commonly used approach in angle-resolved photoemission spectroscopy (ARPES) experiments, due to the possibility to stabilize and tune novel electronic states with properties that can significantly differ from those of the pristine material
By utilizing photon energy-dependent angle-resolved photoemission spectroscopy (ARPES), we have investigated the electronic structure of this material as a function of potassium (K) deposition
Our work provides a reference point for the increasingly popular studies of the alkali metal dosing of semimetals using ARPES
Summary
Alkali metal deposition on layered materials has turned into a commonly used approach in angle-resolved photoemission spectroscopy (ARPES) experiments, due to the possibility to stabilize and tune novel electronic states with properties that can significantly differ from those of the pristine material. In the semiconducting black phosphorus, the band gap was tuned via K dosing, prompting the emergence of Dirac fermions due to the surface Stark effect [2,3,4,5]. This effect has been announced as a universal mechanism of band-gap engineering in 2D semiconductors [6]. The most familiar scenario is “band bending” where a strong variation of the electrostatic potential near the surface
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