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Register a new userDimensional cross-over of the charge density wave order parameter in thin exfoliated 1T-VSe$_2$
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\\'Arp\\'ad P\\'asztor
Publication date
2017
fields
Physics
and research's language is
English
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The capability to isolate one to few unit-cell thin layers from the bulk matrix of layered compounds opens fascinating prospects to engineer novel electronic phases. However, a comprehensive study of the thickness dependence and of potential extrinsic effects are paramount to harness the electronic properties of such atomic foils. One striking example is the charge density wave (CDW) transition temperature in layered dichalcogenides whose thickness dependence remains unclear in the ultrathin limit. Here we present a detailed study of the thickness and temperature dependences of the CDW in VSe$_2$ by scanning tunnelling microscopy (STM). We show that mapping the real-space CDW periodicity over a broad thickness range unique to STM provides essential insight. We introduce a robust derivation of the local order parameter and transition temperature based on the real space charge modulation amplitude. Both quantities exhibit a striking non-monotonic thickness dependence that we explain in terms of a 3D to 2D dimensional crossover in the FS topology. This finding highlights thickness as a true tuning parameter of the electronic ground state and reconciles seemingly contradicting thickness dependencies determined in independent transport studies.
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Metallization of 1T-TaS2 is generally initiated at the domain boundary of charge density wave (CDW), at the expense of its long-range order. However, we demonstrate in this study that the metallization of 1T-TaS2 can be also realized without breaking the long-range CDW order upon surface alkali doping. By using scanning tunneling microscopy, we find the long-range CDW order is always persisting, and the metallization is instead associated with additional in-gap excitations. Interestingly, the in-gap excitation is near the top of the lower Hubbard band, in contrast to a conventional electron-doped Mott insulator where it is beneath the upper Hubbard band. In combination with the numerical calculations, we suggest that the appearance of the in-gap excitations near the lower Hubbard band is mainly due to the effectively reduced on-site Coulomb energy by the adsorbed alkali ions.
How magnetism emerges in low-dimensional materials such as transition metal dichalcogenides at the monolayer limit is still an open question. Herein, we present a comprehensive study of the magnetic properties of single crystal and monolayer VSe$_{2}$, both experimentally and emph{ab initio}. Magnetometry, X-ray magnetic circular dichrosim (XMCD) and emph{ab initio} calculations demonstrate that the charge density wave in bulk stoichiometric VSe$_{2.0}$ causes a structural distortion with a strong reduction in the density of sates at the Fermi level, prompting the system towards a non-magnetic state but on the verge of a ferromagnetic instability. In the monolayer limit, the structural rearrangement induces a Peierls distortion with the opening of an energy gap at the Fermi level and the absence of magnetic order. Control experiments on defect-induced VSe$_{2-delta}$ single crystals show a breakdown of magnetism, discarding vacancies as a possible origin of magnetic order in VSe$_{2}$.
We report a detailed study of the microscopic effects of Cu intercalation on the charge density wave (CDW) in 1textit{T}-Cu$_x$TiSe$_2$. Scanning tunneling microscopy and spectroscopy (STM/STS) reveal a unique, Cu driven spatial texturing of the charge ordered phase, with the appearance of energy dependent CDW patches and sharp $pi$-phase shift domain walls ($pi$DWs). The energy and doping dependencies of the patchwork are directly linked to the inhomogeneous potential landscape due to the Cu intercalants. They imply a CDW gap with unusual features, including a large amplitude, the opening below the Fermi level and a shift to higher binding energy with electron doping. Unlike the patchwork, the $pi$DWs occur independently of the intercalated Cu distribution. They remain atomically sharp throughout the investigated phase diagram and occur both in superconducting and non-superconducting specimen. These results provide unique atomic-scale insight on the CDW ground state, questioning the existence of incommensurate CDW domain walls and contributing to understand its formation mechanism and interplay with superconductivity.
Single layers of transition metal dichalcogenides (TMDCs) are excellent candidates for electronic applications beyond the graphene platform; many of them exhibit novel properties including charge density waves (CDWs) and magnetic ordering. CDWs in these single layers are generally a planar projection of the corresponding bulk CDWs because of the quasi-two-dimensional nature of TMDCs; a different CDW symmetry is unexpected. We report herein the successful creation of pristine single-layer VSe$_2$, which shows a ($sqrt7 times sqrt3$) CDW in contrast to the (4 $times$ 4) CDW for the layers in bulk VSe$_2$. Angle-resolved photoemission spectroscopy (ARPES) from the single layer shows a sizable ($sqrt7 times sqrt3$) CDW gap of $sim$100 meV at the zone boundary, a 220 K CDW transition temperature twice the bulk value, and no ferromagnetic exchange splitting as predicted by theory. This robust CDW with an exotic broken symmetry as the ground state is explained via a first-principles analysis. The results illustrate a unique CDW phenomenon in the two-dimensional limit.
We have investigated the chiral charge-density wave (CDW) in $1T$-VSe$_2$ using scanning tunneling microscopy (STM) measurements and optical polarimetry measurements. With the STM mesurements, we revealed that the CDW intensities along each triple-$q$ directions are different. Thus the rotational symmetry of $1T$-VSe$_2$ is lower than that in typical two-dimentional triple-$q$ CDWs. We found that the CDW peaks form a kagome lattice rather than a triangular lattice. The Friedel oscillations have the chirality and the periodicity reflected properties of the background CDW. With the optical measurements in $1T$-VSe$_2$, we also observed a lower rotational symmetry with the polarization dependence of the transient reflectivity variation, which is consistent with the STM result on a microscopic scale. Both $1T$-TiSe$_2$ and $1T$-VSe$_2$ show chiral CDWs, which implies that such waves are usual for CDWs with the condition $H_mathrm{CDW} equiv q_{1}cdot(q_{2} times q_{3}) eq0$.
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