arXiv subjects

László Forró

Publications and source records attributed to László Forró.

At least 37 records · Page 2Linked to original sources

arXiv2022

Origin of subgap states in normal-insulator-superconductor van der Waals heterostructures

Superconductivity in van der Waals materials, such as NbSe$_{2}$ and TaS$_{2}$, is fundamentally novel due to the effects of dimensionality, crystal symmetries, and strong spin-orbit coupling. In this work we perform tunnel spectroscopy on NbSe$_{2}$ by utilizing MoS$_{2}$ or hexagonal Boron Nitride (hBN) as a tunnel barrier. We observe subgap excitations and probe their origin by studying various heterostructure designs. We show that the edge of NbSe$_{2}$ hosts many defect states, which strongly couple to the superconductor and form Andreev bound states. Furthermore, by isolating the NbSe$_{2}$ edge we show that the subgap states are ubiquitous in MoS$_{2}$ tunnel barriers, but absent in hBN tunnel barriers, suggesting defects in MoS$_{2}$ as their origin. Their magnetic nature reveals a singlet or a doublet type ground state and based on nearly vanishing g-factors or avoided-crossing of subgap excitations we highlight the role of strong spin-orbit coupling.

cond-mat.mes-hall↗

arXiv2022

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↗

arXiv2021

Synthesis of Murunskite Single Crystals: A Bridge Between Cuprates and Pnictides

Numerous contemporary investigations in condensed matter physics are devoted to high temperature (high-$T_c$ ) cuprate superconductors. Despite its unique effulgence among research subjects, the enigma of the high-$T_c$ mechanism still persists. One way to advance its understanding is to discover and study new analogous systems. Here we begin a novel exploration of the natural mineral murunskite, K$_2$FeCu$_3$S$_4$, as an interpolation compound between cuprates and ferropnictides, the only known high-$T_c$ superconductors at ambient pressure. Because in-depth studies can be carried out only on single crystals, we have mastered the synthesis and growth of high quality specimens. Similar to the cuprate parent compounds, these show semiconducting behavior in resistivity and optical transmittance, and an antiferromagnetic ordering at 100 K. Spectroscopy (XPS) and calculations (DFT) concur that the sulfur 3$p$ orbitals are partially open, making them accessible for charge manipulation, which is a prerequisite for superconductivity in analogous layered structures. DFT indicates that the valence band is more cuprate-like, while the conduction band is more pnictide-like. With appropriate doping strategies, this parent compound promises exciting future developments.

cond-mat.mtrl-sci↗

arXiv2021

Three-dimensionally Enlarged Photoelectrodes by a Protogenetic Inclusion of Vertically Aligned Carbon Nanotubes into CH3NH3PbBr3 Single Crystals

We demonstrate that single crystals of methylammonium lead bromide (MAPbBr3) could be grown directly on vertically aligned carbon nanotube (VACNT) forests. The fast-growing MAPbBr3 single crystals engulfed the protogenetic inclusions in the form of individual CNTs, thus resulting in a three-dimensionally enlarged photosensitive interface. Photodetector devices were obtained, detecting low light intensities (~20 nW) from UV range to 550 nm. Moreover, a photocurrent was recorded at zero external bias voltage which points to the plausible formation of a p-n junction resulting from interpenetration of MAPbBr3 single crystals into the VACNT forest. This reveals that vertically aligned CNTs can be used as electrodes in operationally stable perovskite-based optoelectronic devices and can serve as a versatile platform for future selective electrode development.

cond-mat.mtrl-sci↗

arXiv2021

Ultrasensitive 3D Aerosol-Jet-Printed Perovskite X-Ray Photodetector

X-ray photon detection is important for a wide range of applications. The highest demand, however, comes from medical imaging, which requires cost-effective, high-resolution detectors operating at low photon flux, therefore stimulating the search for novel materials and new approaches. Recently, hybrid halide perovskite CH3NH3PbI3 (MAPbI3) has attracted considerable attention due to its advantageous optoelectronic properties and low fabrication costs. The presence of heavy atoms, providing a high scattering cross-section for photons, makes this material a perfect candidate for X-ray detection. Despite the already-successful demonstrations of efficiency in detection, its integration into standard microelectronics fabrication processes is still pending. Here, we demonstrate a promising method for building X-ray detector units by 3D aerosol jet printing with a record sensitivity of 2.2 x 108 μC Gyair-1cm-2 when detecting 8 keV photons at dose-rates below 1 Gy/s (detection limit 0.12 Gy/s), a four-fold improvement on the best-in-class devices. An introduction of MAPbI3-based detection into medical imaging would significantly reduce health hazards related to the strongly ionizing X-rays photons.

cond-mat.mtrl-sci↗

arXiv2021

Light-Emitting Electrochemical Cells of Single Crystal Hybrid Halide Perovskite with Vertically Aligned Carbon Nanotubes Contacts

Based on the reported ion migration under electric field in hybrid lead halide perovskites we have developed a bright, light emitting electrochemical cell with CH3NH3PbBr3 single crystals directly grown on vertically aligned carbon nanotube (VACNT) forests as contact electrodes. Under the applied electric field, charged ions in the crystal drift and accumulate in the vicinity of the electrodes, resulting in an in operando formed p-i-n heterojunction. The decreased interface energy barrier and the strong charge injection due to the CNT tip enhanced electric field, result in a bright green light emission up to 1800 cd/m2 at room temperature (average = 60 cd/m2). Beyond the light emission, this original device architecture points to the possibility of implementing vertically aligned CNTs as electrodes in operationally-stable perovskite-based optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2021

Influence of the organic cation disorder on photoconductivity in ethylenediammonium lead iodide, NH3CH2CH2NH3PbI4

We report the synthesis and crystal structure of an organic inorganic compound, ethylenediammonium lead iodide, NH3CH2CH2NH3PbI4. Synchrotron based single crystal X-ray diffraction experiments revealed that the pristine and thermally treated crystals differ in the organic cation behaviour, which is characterized by a partial disorder in the thermally treated crystal. Based on current voltage measurements, increased disorder of the organic cation is associated with enhanced photoconductivity. This compound could be a potential candidate for interface engineering in lead halide perovskite-based optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2021

Unidirectional Kondo scattering in layered NbS2

Crystalline defects can modify quantum interactions in solids, causing unintuitive, even favourable, properties such as quantum Hall effect or superconducting vortex pinning. Here we present another example of this notion - an unexpected unidirectional Kondo scattering in single crystals of 2H-NbS2. This manifests as a pronounced low-temperature enhancement in the out-of-plane resistivity and thermopower below 40 K, hidden for the in-plane charge transport. The anomaly can be suppressed by the c-axis-oriented magnetic field, but is unaffected by field applied along the planes. The magnetic moments originate from layers of 1T-NbS2, which inevitably form during the growth, undergoing a charge-density-wave reconstruction with each superlattice cell (David-star-shaped cluster of Nb atoms) hosting a localised spin. Our results demonstrate the unique and highly anisotropic response of a spontaneously formed Kondo lattice heterostructure, intercalated in a layered conductor.

cond-mat.str-el↗

arXiv2021

Acoustic-pressure-assisted engineering of aluminium foams

Foaming metals modulates their physical properties, enabling attractive applications where lightweight, low thermal conductivity or acoustic isolation are desirable. Adjusting the size of the bubbles in the foams is particularly relevant for targeted applications. Here we provide a method with a detailed theoretical understanding how to tune the size of the bubbles in aluminium melts in-situ via acoustic pressure. Our description is in full agreement with the high-rate three-dimensional X-Ray radioscopy of the bubble formation. We complement our study with the intriguing results on the effect of foaming on electrical resistivity, Seebeck coefficient and thermal conductivity from cryogenic to room temperature. Compared to bulk materials the investigated foam shows an enhancement in the thermoelectric figure of merit. These results herald promising application of foaming in thermoelectrics materials and devices for thermal energy conversion.

cond-mat.mtrl-sci↗

arXiv2021

Giant anisotropic magnetoresistance in Ising superconductor-magnetic insulator tunnel junctions

Superconductivity and magnetism are generally incompatible because of the opposing requirement on electron spin alignment. When combined, they produce a multitude of fascinating phenomena, including unconventional superconductivity and topological superconductivity. The emergence of two-dimensional (2D)layered superconducting and magnetic materials that can form nanoscale junctions with atomically sharp interfaces presents an ideal laboratory to explore new phenomena from coexisting superconductivity and magnetic ordering. Here we report tunneling spectroscopy under an in-plane magnetic field of superconductor-ferromagnet-superconductor (S/F/S) tunnel junctions that are made of 2D Ising superconductor NbSe2 and ferromagnetic insulator CrBr3. We observe nearly 100% tunneling anisotropic magnetoresistance (AMR), that is, difference in tunnel resistance upon changing magnetization direction from out-of-plane to inplane. The giant tunneling AMR is induced by superconductivity, particularly, a result of interfacial magnetic exchange coupling and spin-dependent quasiparticle scattering. We also observe an intriguing magnetic hysteresis effect in superconducting gap energy and quasiparticle scattering rate with a critical temperature that is 2 K below the superconducting transition temperature. Our study paves the path for exploring superconducting spintronic and unconventional superconductivity in van der Waals heterostructures.

cond-mat.supr-con↗

arXiv2020

Giant anomalous Hall effect in quasi-two-dimensional layered antiferromagnet Co$_{1/3}$NbS$_2$

The discovery of the anomalous Hall effect (AHE) in bulk metallic antiferromagnets (AFMs) motivates the search of the same phenomenon in two-dimensional (2D) systems, where a quantized anomalous Hall conductance can in principle be observed. Here, we present experiments on micro-fabricated devices based on Co$_{1/3}$NbS$_2$, a layered AFM that was recently found to exhibit AHE in bulk crystals below the Néel temperature T$_N$ = 29 K. Transport measurements reveal a pronounced resistivity anisotropy, indicating that upon lowering temperature the electronic coupling between individual atomic layers is increasingly suppressed. The experiments also show an extremely large anomalous Hall conductivity of approximately 400 S/cm, more than one order of magnitude larger than in the bulk, which demonstrates the importance of studying the AHE in small exfoliated crystals, less affected by crystalline defects. Interestingly, the corresponding anomalous Hall conductance, when normalized to the number of contributing atomic planes, is $\sim \, 0.6 \; e^2/h$ per layer, approaching the value expected for the quantized anomalous Hall effect. The observed strong anisotropy of transport and the very large anomalous Hall conductance per layer make the properties of Co$_{1/3}$NbS$_2$ compatible with the presence of partially filled topologically non-trivial 2D bands originating from the magnetic superstructure of the antiferromagnetic state. Isolating atomically thin layers of this material and controlling their charge density may therefore provide a viable route to reveal the occurrence of the quantized AHE in a 2D AFM.

cond-mat.mes-hall↗

arXiv2020

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↗

arXiv2020

Unexpected two-fold symmetric superconductivity in few-layer NbSe$_2$

Two-dimensional transition metal dichalcogenides (TMDs) have been attracting significant interest due to a range of properties, such as layer-dependent inversion symmetry, valley-contrasted Berry curvatures, and strong spin-orbit coupling (SOC). Of particular interest is niobium diselenide (NbSe2), whose superconducting state in few-layer samples is profoundly affected by an unusual type of SOC called Ising SOC. Combined with the reduced dimensionality, the latter stabilizes the superconducting state against magnetic fields up to ~35 T and could lead to other exotic properties such as nodal and crystalline topological superconductivity. Here, we report transport measurements of few-layer NbSe$_2$ under in-plane external magnetic fields, revealing an unexpected two-fold rotational symmetry of the superconducting state. In contrast to the three-fold symmetry of the lattice, we observe that the magnetoresistance and critical field exhibit a two-fold oscillation with respect to an applied in-plane magnetic field. We find similar two-fold oscillations deep inside the superconducting state in differential conductance measurements on NbSe$_2$/CrBr$_3$ superconductor-magnet junctions. In both cases, the anisotropy vanishes in the normal state, demonstrating that it is an intrinsic property of the superconducting phase. We attribute the behavior to the mixing between two closely competing pairing instabilities, namely, the conventional s-wave instability typical of bulk NbSe$_2$ and an unconventional d- or p-wave channel that emerges in few-layer NbSe2. Our results thus demonstrate the unconventional character of the pairing interaction in a few-layer TMD, opening a new avenue to search for exotic superconductivity in this family of 2D materials.

cond-mat.supr-con↗

arXiv2020

Patterns and driving forces of dimensionality-dependent charge density waves in 2H-type transition metal dichalcogenides

Two-dimensional (2D) materials have become a fertile playground for the exploration and manipulation of novel collective electronic states. Recent experiments have unveiled a variety of robust 2D orders in highly-crystalline materials ranging from magnetism to ferroelectricity and from superconductivity to charge density wave (CDW) instability. The latter, in particular, appears in diverse patterns even within the same family of materials with isoelectronic species. Furthermore, how they evolve with dimensionality has so far remained elusive. Here we propose a general framework that provides a unfied picture of CDW ordering in the 2H polytype of four isoelectronic transition metal dichalcogenides 2H-MX$_2$ (M=Nb, Ta and X=S, Se). We first show experimentally that whilst NbSe$_2$ exhibits a strongly enhanced CDW order in the 2D limit, the opposite trend exists for TaSe$_2$ and TaS$_2$, with CDW being entirely absent in NbS$_2$ from its bulk to the monolayer. Such distinct behaviours are then demonstrated to be the result of a subtle, yet profound, competition between three factors: ionic charge transfer, electron-phonon coupling, and the spreading extension of the electronic wave functions. Despite its simplicity, our approach can, in essence, be applied to other quasi-2D materials to account for their CDW response at different thicknesses, thereby shedding new light on this intriguing quantum phenomenon and its underlying mechanisms.

cond-mat.mtrl-sci↗

arXiv2019

Persistent antiferromagnetic order in heavily overdoped Ca$_{1-x}$La$_x$FeAs$_2$

In the Ca$_{1-x}$La$_x$FeAs$_2$ (112) family of pnictide superconductors, we have investigated a highly overdoped composition (x = 0.56), prepared by high-pressure, high-temperature synthesis. Magnetic measurements show an antiferromagnetic transition at TN = 120K, well above the one at lower doping (0.15 < x < 0.27). Below the onset of long-range magnetic order at TN, the electrical resistivity is strongly reduced and is dominated by electron-electron interactions, as evident from its temperature dependence. The Seebeck coefficient shows a clear metallic behavior as in narrow band conductors. The temperature dependence of the Hall coefficient and the violation of Kohler's rule agree with the multiband character of the material. No superconductivity was observed down to 1.8 K. The success of the high-pressure synthesis encourages further investigations of the so far only partially explored phase diagram in this family of Iron-based high temperature superconductors.

cond-mat.mtrl-sci↗

arXiv2019

Electrical transport in onion-like carbon - PMMA nanocomposites

We report electrical conductivity measurements of Polymethyl-methacrylate filled by onion-like carbon particles with primary particle size of $\approx 5$ nm. We shown that the conductivity $σ$ is exceptionally high even at very low loadings, and that its low-temperature dependence follows a Coulomb gap regime at atmospheric pressure and an activated behavior at a pressure of $2$ GPa. We interpret this finding in terms of the enhancement under the applied pressure of the effective dielectric permittivity within the aggregates of onion-like carbons, which improves the screening of the Coulomb interaction and reduces the optimal hopping distance of the electrons.

cond-mat.dis-nn↗

arXiv2018

An unusual continuous paramagnetic-limited superconducting phase transition in 2D NbSe$_2$

Time reversal and spatial inversion are two key symmetries for conventional Bardeen-Cooper-Schrieffer (BCS) superconductivity. Breaking inversion symmetry can lead to mixed-parity Cooper pairing and unconventional superconducting properties. Two-dimensional (2D) NbSe$_2$ has emerged as a new non-centrosymmetric superconductor with the unique out-of-plane or Ising spin-orbit coupling (SOC). Here, we report the observation of an unusual continuous paramagnetic-limited superconductor-normal metal transition in 2D NbSe$_2$. Using tunneling spectroscopy under high in-plane magnetic fields, we observe a continuous closing of the superconducting gap at the upper critical field at low temperatures, in stark contrast to the abrupt first-order transition observed in BCS thin film superconductors. The paramagnetic-limited continuous transition arises from a large spin susceptibility of the superconducting phase due to the Ising SOC. The result is further supported by self-consistent mean-field calculations based on the ab initio band structure of 2D NbSe$_2$. Our findings establish 2D NbSe$_2$ as a promising platform for exploring novel spin-dependent superconducting phenomena and device concepts, such as equal-spin Andreev reflection and topological superconductivity.

cond-mat.supr-con↗

arXiv2018

Magnetic excitations and amplitude fluctuations in insulating cuprates

We present results from light scattering experiments on three insulating antiferromagnetic cuprates, YBa$_2$Cu$_3$O$_{6.05}$, Bi$_2$Sr$_2$YCu$_2$O$_{8+δ}$, and La$_2$CuO$_4$ as a function of polarization and excitation energy {using samples of the latest generation. From the raw data we derive symmetry-resolved spectra.} The spectral shape in $B_{1g}$ symmetry is found to be nearly universal and independent of the excitation energy. The spectra agree quantitatively with predictions by field theory [\onlinecite{Weidinger:2015}] facilitating the precise extraction of the Heisenberg coupling $J$. {In addition, the asymmetric line shape on the high-energy side is found to be related to amplitude fluctuations of the magnetization. In La$_2$CuO$_4$ alone minor contributions from resonance effects may be identified.} The spectra in the other symmetries are not universal. The variations may be traced back to weak resonance effects and extrinsic contributions. For all three compounds we find support for the existence of chiral excitations appearing as a continuum in $A_{2g}$ symmetry having an onset slightly below $3J$. In La$_2$CuO$_4$ an additional isolated excitation appears on top of the $A_{2g}$ continuum.

cond-mat.str-el↗