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Aleš Cahlík

Publications and source records attributed to Aleš Cahlík.

14 recordsLinked to original sources

Emergent ferromagnetism in the NiI$_2$-NbSe$_2$ van der Waals heterostructure

Multiferroicity arising from non-collinear spin textures and strong spin-orbit interactions offers a route to magnetoelectric functionality in the monolayer limit. Although theory predicts that the properties of monolayer multiferroics can be tuned by strain, gating, or proximity effects, experimental demonstrations of such control remain scarce. Here we show that the magnetic ground state of monolayer NiI$_2$, a prototypical two-dimensional multiferroic, is altered by proximity to a superconducting NbSe$_2$ substrate. Using low-temperature scanning tunnelling microscopy (STM) and spectroscopy (STS), we show that the metallic substrate renormalizes the exchange interactions within NiI$_2$ and drives it into a ferromagnetic ground state. This can be visualized by probing the Yu-Shiba-Rusinov (YSR) states within the superconducting gap of the NbSe$_2$ substrate. Our results establish YSR states as an in situ probe of two-dimensional magnetism and demonstrate substrate engineering as a means of controlling magnetic order in atomically thin materials.

cond-mat.mes-hall↗

Interlayer interactions reshape charge-density wave through electronic elasticity in 4H$_{\mathrm{b}}$-TaS$_2$

Incommensurate charge-density waves (CDWs) in layered quantum materials frequently exhibit widely varying ordering wave vectors, even among nominally identical samples, obscuring their intrinsic electronic properties. Here we identify an inherent origin of this variability through the electronic elasticity of an incommensurate CDW using the model heterostructure 4H$_{\mathrm{b}}$-TaS$_2$, composed of alternating commensurate CDW on 1T and incommensurate CDW on 1H layers. Low-temperature scanning tunneling microscopy, combined with Fourier and quasiparticle-interference analysis, exploits the lattice-pinned 1T CDW as an internal reference to resolve discrete compressive ($-2.3\%$) and tensile ($+3.2\%$) elastic states of the neighboring 1H CDW selected by the interlayer registry of the adjacent layers. Corresponding few-meV shifts of a flat band demonstrate that weak interlayer interactions reshape the low-energy electronic structure through the intrinsic elasticity of the incommensurate CDW. These findings establish electronic elasticity as a mechanism by which subtle interlayer interactions control correlated electronic states in van der Waals heterostructures.

cond-mat.str-el↗

Universality of Type-II Multiferroicity in Monolayer Nickel Dihalides

The recent discovery of type-II multiferroicity in monolayer NiI${_2}$ indicated a new pathway for intrinsic magnetoelectric coupling in the two-dimensional limit. However, determining whether this phenomenon is a unique anomaly or a general, chemically tunable property of the material class remains unresolved. Here, we demonstrate the universality of type-II multiferroicity in the transition metal dihalides by visualizing the ferroelectric order in monolayer NiBr${_2}$. Using scanning tunneling microscopy (STM), we resolve atomic-scale ferroelectric domains and confirm their magnetoelectric origin through reciprocal manipulation experiments: reorienting magnetic order via electric fields and suppressing the electric polarization with external magnetic fields. Furthermore, we find that the multiferroic state in NiBr${_2}$ is energetically less robust than in its iodide counterpart, consistent with modified superexchange interactions and the reduced spin-orbit coupling. Our results establish the transition metal dihalides as a versatile platform where the stability of magnetoelectric phases can be engineered through chemical substitution.

cond-mat.mtrl-sci↗

Moiré modulated quantum spin liquid candidate 1T-TaSe$_2$

Quantum spin liquids are quantum phases of matter featuring collectively entangled states and emergent fractional many-body excitations. While methods exist to probe three-dimensional quantum spin liquids experimentally, these techniques lack the sensitivity to probe two-dimensional quantum spin liquids. This seriously hampers the study of potential monolayer quantum spin liquid candidates such as $α$-RuCl$_3$ and 1T-TaSe$_2$. Scanning tunneling microscopy (STM) and spectroscopy (STS) have recently been suggested as promising probes of the quantum spin liquid state, as they can access the spinon spectrum through inelastic tunneling spectroscopy (IETS). In this work, we employ this approach on the quantum spin liquid candidate material 1T-TaSe$_2$ and directly measure its low-energy inelastic excitations. We observe the emergence of a $\sqrt{3}\times\sqrt{3}$ reconstruction driven by the substrate, equivalent spectroscopy across all spin sites and coexistence of zero and finite energy excitations. We show that these observations are consistent with a modulated $\sqrt{3}\times\sqrt{3}$ spin liquid ground state. Our results demonstrate that IETS provides a powerful route to obtain atomic-scale insight into the magnetic excitations of two-dimensional materials, allowing to explore the effects of moiré modulations on potential quantum liquid phases.

cond-mat.str-el↗

Clip-on lens for scanning tunneling luminescence microscopy

We demonstrate and verify the in-situ addition of a collecting lens for electroluminescence experiments to an existing scanning tunneling microscope. We fabricate a simple clip-on lens that we reversibly attach at the sample plate via regular sample transfer tools to collimate the light emitted from a plasmonic tunneling junction to the viewport ordinarily used for optical access. The proximity of the lens to the tunneling junction allows us to exploit the full numerical aperture which helps us achieve good collection efficiencies, demonstrating the quick turnaround of converting an existing setup with optical access into a practical scanning luminescence microscope. We verify the function of the clip-on lens by measuring the bias dependent plasmon of Au, Ag, and spatial luminescence maps.

cond-mat.mes-hall↗

Vacuum cleaving of superconducting niobium tips to optimize noise filtering and with adjustable gap size for scanning tunneling microscopy

Superconducting (SC) tips for scanning tunneling microscopy (STM) can enhance a wide range of surface science studies because they offer exquisite energy resolution, allow the study of Josephson tunneling, or provide spatial contrast based on the local interaction of the SC tip with the sample. The appeal of a SC tip is also practical. An SC gap can be used to characterize and optimize the noise of a low-temperature apparatus. Unlike typical samples, SC tips can be made with less ordered materials, such as from SC polycrystalline wires or by coating a normal metal tip with a superconductor. Those recipes either require additional laboratory infrastructure or are carried out in ambient conditions, leaving an oxidized tip behind. Here, we revisit the vacuum cleaving of an Nb wire to prepare fully gapped tips in an accessible one-step procedure. To show their utility, we measure the SC gap of Nb on Au(111) to determine the base temperature of our microscope and to optimize its RF filtering. The deliberate coating of the Nb tip with Au fully suppresses the SC gap and we show how sputtering with Ar$^{+}$ ions can be used to gradually recover the gap, promising tunability for tailored SC gaps sizes.

cond-mat.supr-con↗

A versatile platform for graphene nanoribbon synthesis, electronic decoupling, and spin polarized measurements

The on-surface synthesis of nano-graphenes has led the charge in prototyping structures with perspectives beyond silicon-based technology. Following reports of open-shell systems in graphene-nanoribbons (GNR), a flurry of research activities is directed at investigating their magnetic properties with a keen eye for spintronic applications. Although the synthesis of nano-graphenes is usually straightforward on gold, it is difficult to use it for electronic decoupling and spin-polarized measurements. Using a binary alloy Cu3Au(111), we show how to combine the efficient gold-like nano-graphene formation with spin polarization and electronic decoupling known from copper. We prepare copper oxide layers, demonstrate thermally and tip-assisted synthesis of GNR and grow thermally stable magnetic Co islands. We functionalize the tip of a scanning tunneling microscope with carbon-monoxide, nickelocene, or attach Co clusters for high-resolution imaging, magnetic sensing, or spin-polarized measurements. This versatile platform will be a valuable tool in the advanced study of magnetic nano-graphenes.

cond-mat.mes-hall↗

A Sacrificial Magnet Concept for Field Dependent Surface Science Studies

We demonstrate a straightforward approach to integrating a magnetic field into a low-temperature scanning tunneling microscope (STM) by adhering an NdFeB permanent magnet to a magnetizable sample plate. To render our magnet concept compatible with high-temperature sample cleaning procedures, we make the irreversible demagnetization of the magnet a central part of our preparation cycle. After sacrificing the magnet by heating it above its Curie temperature, we use a transfer tool to attach a new magnet in-situ prior to transferring the sample into the STM. We characterize the magnetic field created by the magnet using the Abrikosov vortex lattice of superconducting NbSe2. Excellent agreement between the distance dependent magnetic fields from experiments and simulations allows us to predict the magnitude and orientation of magnetic flux at any location with respect to the magnet and the sample plate. Our concept is an accessible solution for field-dependent surface science studies that require fields in the range of up to 400 mT and otherwise detrimental heating procedures.

physics.app-ph↗

Counting Molecules: Python based scheme for automated enumeration and categorization of molecules in scanning tunneling microscopy images

Scanning tunneling and atomic force microscopies (STM/nc-AFM) are rapidly progressing to offer unprecedented spatial resolution of a diverse array of chemical species. In particular, they are employed to characterize on-surface chemical reactions by directly examining precursors and products. Chiral effects and self-assembled structures can also be investigated. This open source, modular, python based scheme automates the categorization of a variety of molecules present in medium sized (10$\times$10 to 100$\times$100 nm) scanned probe images.

cond-mat.mes-hall↗

The Role of the Magnetic Anisotropy in Atomic-Spin Sensing of 1D Molecular Chains

One-dimensional metal-organic chains often possess a complex magnetic structure susceptible to be modified by a alteration of their chemical composition. The possibility to tune their magnetic properties provides an interesting playground to explore quasiparticle interactions in low-dimensional systems. Despite the great effort invested so far, a detailed understanding of the interactions governing the electronic and magnetic properties of the low-dimensional systems is still incomplete. One of the reasons is the limited ability to characterize their magnetic properties at the atomic scale. Here, we provide a comprehensive study of the magnetic properties of metal-organic one-dimensional (1D) coordination polymers consisting of 2,5-diamino-1,4-benzoquinonediimine ligands coordinated with Co or Cr atoms synthesized in ultra-high vacuum conditions on a Au(111) surface. A combination of an integral X-ray spectroscopy with local-probe inelastic electron tunneling spectroscopy corroborated by multiplet analysis, density functional theory, and inelastic electron tunneling simulations enable us to obtain essential information about their magnetic structure, including the spin magnitude and orientation at the magnetic atoms, as well as the magnetic anisotropy.

cond-mat.mes-hall↗

Significance of nuclear quantum effects in hydrogen bonded molecular chains

In hydrogen bonded systems, nuclear quantum effects such as zero-point motion and tunneling can significantly affect their material properties through underlying physical and chemical processes. Presently, direct observation of the influence of nuclear quantum effects on the strength of hydrogen bonds with resulting structural and electronic implications remains elusive, leaving opportunities for deeper understanding to harness their fascinating properties. We studied hydrogen-bonded one-dimensional quinonediimine molecular networks which may adopt two isomeric electronic configurations via proton transfer. Herein, we demonstrate that concerted proton transfer promotes a delocalization of π-electrons along the molecular chain, which enhances the cohesive energy between molecular units, increasing the mechanical stability of the chain and giving rise to new electronic in-gap states localized at the ends. These findings demonstrate the identification of a new class of isomeric hydrogen bonded molecular systems where nuclear quantum effects play a dominant role in establishing their chemical and physical properties. We anticipate that this work will open new research directions towards the control of mechanical and electronic properties of low-dimensional molecular materials via concerted proton tunneling.

cond-mat.mes-hall↗

Charge carrier injection electroluminescence with CO functionalized tips on single molecular emitters

We investigate electroluminescence of single molecular emitters on NaCl on Ag(111) and Au(111) with submolecular resolution in a low-temperature scanning probe microscope with tunneling current, atomic force and light detection capabilities. Role of the tip state is studied in the photon maps of a prototypical emitter, zinc phthalocyanine (ZnPc), using metal and CO-metal tips. CO-functionalization is found to have a dramatic impact on the resolution and contrast of the photon maps due to the localized overlap of the p-orbitals on the tip with the molecular orbitals of the emitter. The possibility of using the same CO-functionalized tip for tip-enhanced photon detection and high resolution atomic force is demonstrated. We study the electroluminescence of ZnPc, induced by charge carrier injection at sufficiently high bias voltages. We propose that the distinct level alignment of the ZnPc frontier orbital with the Au(111) and Ag(111) Fermi levels governs the primary excitation mechanisms as the injection of electrons and holes from the tip into the molecule, respectively. These findings put forward the importance of the tip status in the photon maps and contribute to a better understanding of the photophysics of organic molecules on surfaces.

cond-mat.mes-hall↗

Identification of two-dimensional $FeO_2$ termination of hematite $α-Fe_2O_3(0001)$ surface

Iron oxides are among the most abundant compounds on Earth and have consequently been studied and used extensively in industrial processes. Despite these efforts, concrete understanding of some of their surface phase structures has remained elusive, in particular the oxidized $α-Fe_2O_3(0001)$ hematite surface. We detail an optimized recipe to produce this phase over the entire hematite surface and study the geometrical parameters and composition of its complex structure by means of atomically resolved microscopy, electron diffraction and surface-sensitive spectroscopies. We conclude that the oxidized $α-Fe_2O_3(0001)$ surface is terminated by a two-dimensional iron oxide with structure, lattice parameters, and orientation different from the bulk substrate. Using total-energy density functional theory for simulation of a large-scale atomic model, we identify the structure of the surface layer as antiferromagnetic, conductive $1T-FeO_2$ attached on half-metal terminated bulk. The model succeeds in reproducing the characteristic modulations observed in the atomically resolved images and electron diffraction patterns.

cond-mat.mtrl-sci↗

On-Surface Structural and Electronic Properties of Spontaneously Formed Tb$_2$Pc$_3$ Single Molecule Magnets

The single molecule magnet (SMM) bis(phthalocyaninato)terbium (III) (TbPc$_2$) has attracted steady research attention as an exemplar system for realizing molecule-based spin electronics. In this paper, we report on the spontaneous formation of Tb$_2$Pc$_3$ species from TbPc$_2$ precursors via sublimation in ultrahigh vacuum (UHV) onto an Ag(111) surface. The molecules on the surface are inspected using combined scanning tunneling (STM) and non-contact atomic force microscopies (nc-AFM) at 5 Kelvin. Submolecular resolution and height dependent measurements supported by density functional theory (DFT) calculations unambiguously show the presence of both TbPc$_2$ and Tb$_2$Pc$_3$ species. The synthesis of Tb$_2$Pc$_3$ species under UHV conditions is independently confirmed by chemical analysis. The high-resolution AFM imaging allows us to register the orientation of the topmost Pc ligand in both Tb$_2$Pc$_3$ and TbPc$_2$ relative to the underlying Ag(111) surface. Measurements of the electronic structure reveal the selective appearance of a Kondo signature with temperature $\sim$ 30K in the Tb$_2$Pc$_3$ species, localized to the Pc ligand lobes. We attribute the presence of the Kondo resonance on select Tb$_2$Pc$_3$ molecules to the orientation of internal molecular ligands. High-resolution AFM imaging identifies geometric distortions between Tb$_2$Pc$_3$ molecules with and without the Kondo effect, the result of the complex interplay between structural and electronic differences.

cond-mat.mes-hall↗