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Eduard Tutiš

Publications and source records attributed to Eduard Tutiš.

6 recordsLinked to original sources

Intercalation-induced states at the Fermi level and the coupling of intercalated magnetic ions to conducting layers in Ni$_{1/3}$NbS$_2$

The magnetic sublayers introduced by intercalation into the host transition-metal dichalcogenide (TMD) are known to produce various magnetic states. The magnetic sublayers and their magnetic ordering strongly modify the electronic coupling between layers of the host compound. Understanding the roots of this variability is a significant challenge. Here we employ the angle-resolved photoelectron spectroscopy at various photon energies, the {\it ab initio} electronic structure calculations, and modeling to address the particular case of Ni-intercalate, Ni$_{1/3}$NbS$_2$. We find that the bands around the Fermi level bear the signature of a strong yet unusual hybridization between NbS$_2$ conduction band states and the Ni 3$d$ orbitals. The hybridization between metallic NbS$_2$ layers is almost entirely suppressed in the central part of the Brillouin zone, including the part of the Fermi surface around the $\mathrmΓ$ point. Simultaneously, it gets very pronounced towards the zone edges. It is shown that this behavior is the consequence of the rather exceptional, {\it symmetry imposed}, spatially strongly varying, {\it zero total} hybridization between relevant Ni magnetic orbitals and the neighboring Nb orbitals that constitute the metallic bands. We also report the presence of the so-called $β$-feature, discovered only recently in two other magnetic intercalates with very different magnetic orderings. In Ni$_{1/3}$NbS$_2$, the feature shows only at particular photon energies, indicating its bulk origin. Common to prior observations, it appears as a series of very shallow electron pockets at the Fermi level, positioned along the edge of the Brillouin zone. Unforeseen by {\it ab initio} electronic calculations, and its origin still unresolved, the feature appears to be a robust consequence of the intercalation of 2H-NbS$_2$ with magnetic ions.

cond-mat.mtrl-sci↗

Electronic transport and magnetism in the alternating stack of metallic and highly frustrated magnetic layers in Co$_{1/3}$NbS$_2$

Transition-metal dichalcogenides (TMDs) are layered compounds that support many electronic phases, including various charge density waves, superconducting, and Mott insulating states. Their intercalation with magnetic ions introduces magnetic sublayers, which strongly influence the coupling between host layers, and feature various magnetic states adjustable by external means. Co$_{1/3}$NbS$_2$ hosts a particularly sensitive magnetic subsystem with the lowest magnetic ordering temperature in the family of magnetically intercalated TMDs, and the only one where the complete suppression of magnetic order under pressure has been recently suggested. By combining the results of several experimental methods, electronic ab initio calculations, and modeling, we develop insights into the mechanisms of electric transport, magnetic ordering, and their interaction in this compound. The elastic neutron scattering is used to directly follow the evolution of the antiferromagnetic order parameter with pressure and temperature. Our results unambiguously disclose the complete suppression of the observed magnetic order around 1.7 GPa. We delve into possible mechanisms of magnetic order suppression under pressure, highlighting the role of magnetic frustrations indicated by magnetic susceptibility measurements and ab-initio calculations. Electronic conduction anisotropy is measured in the wide temperature and pressure range. Here we show that the transport in directions along and perpendicular to layers respond differently to the appearance of magnetic ordering or the application of the hydrostatic pressure. We propose the 'spin-valve' mechanism where the intercalated Co ions act as spin-selective electrical transport bridges between host layers. The mechanism applies to various magnetic states and can be extended to other magnetically intercalated TMDs.

cond-mat.str-el↗

Role of intercalated Cobalt in the electronic structure of Co$_{1/3}$NbS$_2$

Co$_{1/3}$NbS$_2$ is the magnetic intercalate of 2H-NbS$_2$ where electronic itinerant and magnetic properties strongly influence each other throughout the phase diagram. Here we report the first angle-resolved photoelectron spectroscopy (ARPES) study in Co$_{1/3}$NbS$_2$. The observed electronic structure seemingly resembles the one of the parent material 2H-NbS$_2$, with the shift in Fermi energy of 0.5 eV accounting for the charge transfer of approximately two electrons from each Co ion into the NbS$_2$ layers. However, we observe significant departures from the 2H-NbS$_2$ rigid band picture: Entirely unrelated to the 2H-NbS$_2$ electronic structure, a shallow electronic band is found crossing the Fermi level near the boundary of the first Brillouin zone of the superstructure imposed by the intercalation. The evolution of the experimental spectra upon varying the incident photon energy suggests the Co origin of this band. Second, the Nb bonding band, found deeply submerged below the Fermi level at the $Γ$ point, indicates the interlayer-hybridization being very much amplified by intercalation, with Co magnetic ions probably acting as covalent bridges between NbS$_2$ layers. The strong hybridization between conducting and magnetic degrees of freedom suggests dealing with strongly correlated electron system where the interlayer coupling plays an exquisite role.

cond-mat.str-el↗

Preferential out-of-plane conduction and quasi-one-dimensional electronic states in layered 1T-TaS2

Layered transition metal dichalcogenides (TMDs) are commonly classified as quasi-two-dimensional materials, meaning that their electronic structure closely resembles that of an individual layer, which results in resistivity anisotropies reaching thousands. Here, we show that this rule does not hold for 1T-TaS2 - a compound with the richest phase diagram among TMDs. While the onset of charge density wave order makes the in-plane conduction non-metallic, we reveal that the out-of-plane charge transport is metallic and the resistivity anisotropy is close to one. We support our findings with ab-initio calculations predicting a pronounced quasi-one-dimensional character of the electronic structure. Consequently, we interpret the highly debated metal-insulator transition in 1T-TaS2 as a quasi-one-dimensional instability, contrary to the long-standing Mott localisation picture. In a broader context, these findings are relevant for the newly born field of van der Waals heterostructures, where tuning interlayer interactions (e.g. by twist, strain, intercalation, etc.) leads to new emergent phenomena.

cond-mat.mtrl-sci↗

Semimetallic and charge-ordered $α$-(BEDT-TTF)$_2$I$_3$: on the role of disorder in dc transport and dielectric properties

$α$-(BEDT-TTF)$_2$I$_3$ is a prominent example of charge ordering among organic conductors. In this work we explore the details of transport within the charge-ordered as well as semimetallic phase at ambient pressure. In the high-temperature semimetallic phase, the mobilities and concentrations of both electrons and holes conspire in such a way to create an almost temperature-independent conductivity as well as a low Hall effect. We explain these phenomena as a consequence of a predominantly inter-pocket scattering which equalizes mobilities of the two types of charge carriers. At low temperatures, within the insulating charge-ordered phase two channels of conduction can be discerned: a temperature-dependent activation which follows the mean-field behavior, and a nearest-neighbor hopping contribution. Together with negative magnetoresistance, the latter relies on the presence of disorder. The charge-ordered phase also features a prominent dielectric peak which bears a similarity to relaxor ferroelectrics. Its dispersion is determined by free-electron screening and pushed by disorder well below the transition temperature. The source of this disorder can be found in the anion layers which randomly perturb BEDT-TTF molecules through hydrogen bonds.

cond-mat.str-el↗

Scattering dominated high-temperature phase of 1T-TiSe2: an optical conductivity study

The controversy regarding the precise nature of the high-temperature phase of 1T-TiSe2 lasts for decades. It has intensified in recent times when new evidence for the excitonic origin of the low-temperature charge-density wave state started to unveil. Here we address the problem of the high-temperature phase through precise measurements and detailed analysis of the optical response of 1T-TiSe2 single crystals. The separate responses of electron and hole subsystems are identified and followed in temperature. We show that neither semiconductor nor semimetal pictures can be applied in their generic forms as the scattering for both types of carriers is in the vicinity of the Ioffe-Regel limit with decay rates being comparable to or larger than the offsets of band extrema. The nonmetallic temperature dependence of transport properties comes from the anomalous temperature dependence of scattering rates. Near the transition temperature the heavy electrons and the light holes contribute equally to the conductivity. This surprising coincidence is regarded as the consequence of dominant intervalley scattering that precedes the transition. The low-frequency peak in the optical spectra is identified and attributed to the critical softening of the L-point collective mode.

cond-mat.str-el↗