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Igor Marković

Publications and source records attributed to Igor Marković.

10 recordsLinked to original sources

Nature of the current-induced insulator-to-metal transition in Ca$_2$RuO$_4$ as revealed by transport-ARPES

The Mott insulator Ca$_2$RuO$_4$ exhibits a rare insulator-to-metal transition (IMT) induced by DC current. While structural changes associated with this transition have been tracked by neutron diffraction, Raman scattering, and x-ray spectroscopy, work on elucidating the response of the electronic degrees of freedom is still in progress. Here we unveil the current-induced modifications of the electronic states of Ca$_2$RuO$_4$ by employing angle-resolved photoemission spectroscopy (ARPES) in conjunction with four-probe transport. Two main effects emerge: a clear reduction of the Mott gap and a modification in the dispersion of the Ru-bands. The changes in dispersion occur exclusively along the $XM$ high-symmetry direction, parallel to the $b$-axis where the greatest in-plane lattice change occurs. These experimental observations, together with dynamical mean-field theory (DMFT) calculations simulated from the current-induced structural distortions, indicate the intimate interplay of lattice and orbital-dependent electronic response in the current-driven IMT. Furthermore, based on a free energy analysis, we demonstrate that the current-induced phase, albeit thermodynamically equivalent, is electronically distinct from the high-temperature zero-current metallic phase. Our results provide insight into the elusive nature of the current-induced IMT of Ca$_2$RuO$_4$ and advance the challenging, yet powerful, technique of transport-ARPES.

cond-mat.str-el↗

Charge doping into spin minority states mediates doubling of $T_\mathrm{C}$ in ferromagnetic CrGeTe$_3$

The recent discovery of the persistence of long-range magnetic order when van der Waals layered magnets are thinned towards the monolayer limit has provided a tunable platform for the engineering of novel magnetic structures and devices. Here, we study the evolution of the electronic structure of CrGeTe$_3$ as a function of electron doping in the surface layer. From angle-resolved photoemission spectroscopy, we observe spectroscopic fingerprints that this electron doping drives a marked increase in $T_\mathrm{C}$, reaching values more than double that of the undoped material, in agreement with recent studies using electrostatic gating. Together with density functional theory calculations and Monte Carlo simulations, we show that, surprisingly, the increased $T_\mathrm{C}$ is mediated by the population of spin-minority Cr $t_{2g}$ states, forming a half-metallic 2D electron gas at the surface. We show how this promotes a novel variant of double exchange, and unlocks a significant influence of the Ge -- which was previously thought to be electronically inert in this system -- in mediating Cr-Cr exchange.

cond-mat.mtrl-sci↗

Tuneable electron-magnon coupling of ferromagnetic surface states in PdCoO$_2$

Controlling spin wave excitations in magnetic materials underpins the burgeoning field of magnonics. Yet, little is known about how magnons interact with the conduction electrons of itinerant magnets, or how this interplay can be controlled. Via a surface-sensitive spectroscopic approach, we demonstrate a strong and highly-tuneable electron-magnon coupling at the Pd-terminated surface of the delafossite oxide PdCoO$_2$, where a polar surface charge mediates a Stoner transition to itinerant surface ferromagnetism. We show how the coupling can be enhanced 7-fold with increasing surface disorder, and concomitant charge carrier doping, becoming sufficiently strong to drive the system into a polaronic regime, accompanied by a significant quasiparticle mass enhancement. Our study thus sheds new light on electron-magnon interactions in solid-state materials, and the ways in which these can be controlled.

cond-mat.str-el↗

Hot carrier-assisted switching of the electron-phonon interaction in 1$T$-VSe$_2$

We apply an intense infrared laser pulse in order to perturb the electronic and vibrational states in the three-dimensional charge density wave material 1$T$-VSe$_2$. Ultrafast snapshots of the light-induced hot carrier dynamics and non-equilibrium quasiparticle spectral function are collected using time- and angle-resolved photoemission spectroscopy. The hot carrier temperature and time-dependent electronic self-energy are extracted from the time-dependent spectral function, revealing that incoherent electron-phonon interactions heat the lattice above the charge density wave critical temperature on a timescale of $(200 \pm 40)$~fs. Density functional perturbation theory calculations establish that the presence of hot carriers alters the overall phonon dispersion and quenches efficient low-energy acoustic phonon scattering channels, which results in a new quasi-equilibrium state that is experimentally observed.

cond-mat.mtrl-sci↗

Changes of Fermi Surface Topology due to the Rhombohedral Distortion in SnTe

Stoichiometric SnTe is theoretically a small gap semiconductor that undergoes a ferroelectric distortion on cooling. In reality however, crystals are always non-stoichiometric and metallic; the ferroelectric transition is therefore more accurately described as a polar structural transition. Here we study the Fermi surface using quantum oscillations as a function of pressure. We find the oscillation spectrum changes at high pressure, due to the suppression of the polar transition and less than 10 kbar is sufficient to stabilize the undistorted cubic lattice. This is accompanied by a large decrease in the Hall and electrical resistivity. Combined with our density functional theory (DFT) calculations and angle resolved photoemission spectroscopy (ARPES) measurements this suggests the Fermi surface $L$-pockets have lower mobility than the tubular Fermi surfaces that connect them. Also captured in our DFT calculations is a small widening of the band gap and shift in density of states for the polar phase. Additionally we find the unusual phenomenon of a linear magnetoresistance that exists irrespective of the distortion that we attribute to regions of the Fermi surface with high curvature.

cond-mat.str-el↗

Ultrafast triggering of insulator-metal transition in two-dimensional VSe$_2$

Assembling transition metal dichalcogenides (TMDCs) at the two-dimensional (2D) limit is a promising approach for tailoring emerging states of matter such as superconductivity or charge density waves (CDWs). Single-layer (SL) VSe$_2$ stands out in this regard because it exhibits a strongly enhanced CDW transition with a higher transition temperature compared to the bulk in addition to an insulating phase with an anisotropic gap at the Fermi level, causing a suppression of anticipated 2D ferromagnetism in the material. Here, we investigate the interplay of electronic and lattice degrees of freedom that underpin these electronic phases in SL VSe$_2$ using ultrafast pump-probe photoemission spectroscopy. In the insulating state, we observe a light-induced closure of the energy gap on a timescale of 480 fs, which we disentangle from the ensuing hot carrier dynamics. Our work thereby reveals that the phase transition in SL VSe$_2$ is driven by electron-lattice coupling and demonstrates the potential for controlling electronic phases in 2D materials with light.

cond-mat.mtrl-sci↗

Band hybridisation at the semimetal-semiconductor transition of Ta$_2$NiSe$_5$ enabled by mirror-symmetry breaking

We present a combined study from angle-resolved photoemission and density-functional theory calculations of the temperature-dependent electronic structure in the excitonic insulator candidate Ta$_2$NiSe$_5$. Our experimental measurements unambiguously establish the normal state as a semimetal with a significant band overlap of $>$100~meV. Our temperature-dependent measurements indicate how these low-energy states hybridise when cooling through the well-known 327~K phase transition in this system. From our calculations and polarisation-dependent photoemission measurements, we demonstrate the importance of a loss of mirror symmetry in enabling the band hybridisation, driven by a shear-like structural distortion which reduces the crystal symmetry from orthorhombic to monoclinic. Our results thus point to the key role of the lattice distortion in enabling the phase transition of Ta$_2$NiSe$_5$.

cond-mat.str-el↗

Direct observation of the energy gain underpinning ferromagnetic superexchange in the electronic structure of CrGeTe$_3$

We investigate the temperature-dependent electronic structure of the van der Waals ferromagnet, CrGeTe$_3$. Using angle-resolved photoemission spectroscopy, we identify atomic- and orbital-specific band shifts upon cooling through ${T_\mathrm{C}}$. From these, together with x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we identify the states created by a covalent bond between the Te ${5p}$ and the Cr ${e_g}$ orbitals as the primary driver of the ferromagnetic ordering in this system, while it is the Cr ${t_{2g}}$ states that carry the majority of the spin moment. The ${t_{2g}}$ states furthermore exhibit a marked bandwidth increase and a remarkable lifetime enhancement upon entering the ordered phase, pointing to a delicate interplay between localized and itinerant states in this family of layered ferromagnets.

cond-mat.str-el↗

Momentum-resolved linear dichroism in bilayer MoS$_2$

Inversion-symmetric crystals are optically isotropic and thus naively not expected to show dichroism effects in optical absorption and photoemission processes. Here, we find a strong linear dichroism effect (up to 42.4%) in the conduction band of inversion-symmetric bilayer MoS$_2$, when measuring energy- and momentum-resolved snapshots of excited electrons by time- and angle-resolved photoemission spectroscopy. We model the polarization-dependent photoemission intensity in the transiently-populated conduction band using the semiconductor Bloch equations and show that the observed dichroism emerges from intralayer single-particle effects within the isotropic part of the dispersion. This leads to optical excitations with an anisotropic momentum-dependence in an otherwise inversion symmetric material.

cond-mat.mtrl-sci↗

Orbital- and $k_z$-selective hybridisation of Se 4p and Ti 3d states in the charge density wave phase of TiSe$_2$

We revisit the enduring problem of the $2\times{}2\times{}2$ charge density wave (CDW) order in TiSe$_2$, utilising photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridisation that is strongly $k_z$-dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe$_2$.

cond-mat.str-el↗