arXiv subjects

Denis V. Vyalikh

Publications and source records attributed to Denis V. Vyalikh.

14 recordsLinked to original sources

arXiv2026

Photoemission insights into lanthanide-based crystals

The interplay of strongly localized 4$f$ electrons with itinerant spd-valence states gives rise to a wide range of correlated phenomena and properties that place lanthanide materials at the focus of considerable research efforts. Beyond the bulk, their surfaces are of particular interest, where the reduced coordination, a modified crystal electric field, broken inversion symmetry in combination with strong spin-orbit coupling, and the emergence of surface states and resonances considerably reshape 4$f$-driven electronic and magnetic properties. This, in turn, enables novel functionalities of particular relevance for low-dimensional systems and their applications. This review summarizes how advances in photoelectron spectroscopies, together with improved crystal growth, have enabled detailed insights into bulk and surface phenomena of lanthanide-based crystals. After a brief overview of key developments from the 1970s to the 1990s, we discuss recent progress, focusing on systematic studies by the authors and collaborators that form a coherent line of research. These include the unveiling of $k$-resolved $f-spd$ hybridization, the formation and evolution with temperature of $f$-derived Fermi surface in Kondo lattices, layer-dependent 4$f$ magnetic anisotropy, the emergence of ferromagnetically ordered surfaces in systems with non-magnetic bulk ground state. This coherent line of research addresses core questions in the physics of 4$f$ systems and opens opportunities for engineering novel lanthanide-based architectures, including heterostructures and supramolecular complexes with novel physical properties and functionalities.

cond-mat.str-el↗

arXiv2026

Atomically Thin Amorphous Carbon with an Ultralow Dielectric Constant

Two-dimensional (2D) materials exhibit excellent properties at monolayer thickness and are viable replacements for various microelectronic components as scaling gradually approaches the atomic limit. Despite significant advancements in the ongoing 2D revolution of integrated circuits, one crucial building block, namely a 2D ultralow-k (ULK) dielectric, remains unreported. The challenge lies in achieving a dielectric constant less than 3, as traditional low-k dielectrics are inherently unstable at the 2D limit due to their amorphous or porous nature. The realisation of ultrathin dielectrics with low-k is also needed to address current bottlenecks in integrated circuits scaling. Specifically, low-k materials are necessary to minimise parasitic capacitances as the distance between conductive elements shrinks below 10 nm. Moreover, advanced architectures like gate-all-around field effect transistors (GAA FET) require even lower dielectric constants (k<2) at sub-3nm thickness. Here, we show that layer-by-layer grown multilayer amorphous carbon (ML-AC), as thin as 0.8 nm, is a mechanically robust 2D ULK dielectric with k of 1.35 and dielectric strength of 28-31 MV cm-1. The lack of any long-range order, its intrinsic 2D nature, sp2 carbon character and low density are all essential for minimising dielectric permittivity. Moreover, ML-AC overcomes the vulnerability of existing dielectrics to ion diffusion degradation with a record metal ion diffusion time to failure (TTF) of 10^10 s for even a single layer. Therefore, otherwise necessary additional layers occupying up to 3 nm can be eliminated, which is especially significant as metal line widths approach 10 nm. Combined with its low-temperature, direct and conformal growth even on a dielectric, these critical features enable substantial improvements in silicon-based semiconductor electronics and ensure compatibility with future 2D electronics.

cond-mat.mtrl-sci↗

arXiv2026

Interplay of Kondo Physics with Incommensurate Charge Density Waves in CeTe$_3$

CeTe$_3$ is a 2--dimensional (2D) Van der Waals (VdW) material with incommensurate charge density waves (CDW), extremely high transition temperature ($T_{CDW}$) and a large momentum--dependent CDW gap that leaves a significant portion of the Fermi surface intact. It is also considered to be a weak Kondo system, a property unexpected for a material with incommensurate CDW, where each atomic site is slightly different. Here, we study the properties of the CDW state in several RTe$_3$ (R is rare earth) materials and examine the hybridization of itinerant states with the localized Ce $4f$ multiplet in CeTe$_3$ by using angle resolved photoemission spectroscopy (ARPES). We find that the renormalization of the itinerant states originating from the hybridization with the deeper localized $4f$ states at $-260$ meV is $k-$dependent and extends to the Fermi level. As these localized states are far from the Fermi level, the observed hybridization affects the effective masses only marginally and does not lead to heavy fermions. However, since the same renormalizing mechanism normally leads to the heavy fermion physics when the localized $4f$ states are near the Fermi level, our observation of its strong $k-$dependence suggests that this could be the reason for discrepancy between the heavy masses in specific heat and light ones in Shubnikov de Haas oscillations, often observed in heavy fermions.

cond-mat.str-el↗

arXiv2025

Strongly Entangled Kondo and Kagome Lattices and the Emergent Magnetic Ground State in Heavy-Fermion Kagome Metal YbV$_6$Sn$_6$

Applying angle-resolved photoemission spectroscopy and density functional theory calculations, we present compelling spectroscopic evidence demonstrating the intertwining and mutual interaction between the Kondo and kagome sublattices in heavy-fermion intermetallic compound YbV$_6$Sn$_6$. We reveal the Yb 4$f$-derived states near the Fermi level, along with the presence of bulk kagome bands and topological surface states. We unveil strong interactions between the 4$f$ and itinerant electrons, where the kagome bands hosting the Dirac fermions and van Hove singularities predominate. Such findings are well described using a $c$-$f$ hybridization model. On the other hand, our systematic characterization of magnetic properties demonstrates an unusually enhanced antiferromagnetic ordering, where the kagome-derived van Hove singularities near $E_F$ play a vital role in determining the unconventional nature of the Ruderman-Kittel-Kasuya-Yosida interaction and Kondo coupling. These unique kagome-state-mediated exchange interactions have never been reported before and could lead to a novel phase diagram and various quantum critical behaviors in YbV$_6$Sn$_6$ and its siblings. Our results not only expand the family of exotic quantum phases entangled with kagome structure to the strongly correlated regime, but also establish YbV$_6$Sn$_6$ as an unprecedented platform to explore unconventional many-body physics beyond the standard Kondo picture.

cond-mat.str-el↗

arXiv2025

Orbital-selective band modifications in a charge-ordered kagome metal LuNb$_6$Sn$_6$

The origin of the charge order in kagome lattice materials has attracted great interest due to the unique electronic structure features connected to kagome networks and the interplay between electron and lattice degrees of freedom. Recently, compounds with composition $Ln$Nb$_6$Sn$_6$ ($Ln$ = Ce-Nd, Sm, Gd-Tm, Lu, Y) appear as a new family of kagome metals, structurally analogous to $R$V$_6$Sn$_6$ ($R$ = Sc, Y, or rare earth) systems. Among them, LuNb$_6$Sn$_6$ emerges as a novel material hosting charge density wave (CDW) with a $\sqrt{3}$ $\times$ $\sqrt{3}$ $\times$ $3$ wave vector, akin to that in ScV$_6$Sn$_6$. Here, we employ high-resolution angle-resolved photoemission spectroscopy, scanning tunneling microscopy, and density functional theory calculations to systematically investigate the electronic properties of LuNb$_6$Sn$_6$. Our observation reveals the characteristic band structures of the "166" kagome system. A charge instability driven by Fermi surface nesting is decisively ruled out through an analysis of the interactions between van Hove singularities. Across the CDW transition, we observe orbital-selective band modifications, with noticeable evolutions of Lu 5$d$ and Sn 5$p$ electrons, while Nb 4$d$ electrons exhibit minimal change, suggesting that the Lu and Sn sites other than the Nb kagome lattice play a key role in the formation of CDW. Our findings substantiate a universal lattice-driven CDW mechanism rather than a charge-instability-driven one in the "166" kagome compounds, making it a distinct material class compared to other charge-ordered kagome systems, such as $A$V$_3$Sb$_5$ ($A$ = K, Rb, Cs) and FeGe.

cond-mat.str-el↗

arXiv2025

Magnetic frustration and weak Mn magnetic ordering in EuMn$_2$P$_2$

We report on the electron spin resonance (ESR), heat capacity, magnetization, nuclear magnetic resonance (NMR), magnetic circular and linear dichroism (XMCD, XMLD), as well as the electrical resistivity of EuMn$_{2}$P$_{2}$ single crystals. Antiferromagnetic order of Eu was observed in several quantities at $T^{\rm Eu}_{\rm N}\,=\,18\,\rm K$. The temperature dependencies of ESR linewidth and resonance shift show, when approaching the Eu-ordered state, a divergence towards $T^{\rm Eu}_{\rm N}$, indicating the growing importance of magnetic correlations and the build-up of internal magnetic fields. An additional temperature scale of $\approx 47\,\rm K$ has considerable impact on linewidth, resonance field and intensity. This points to the presence of weak Mn-based ordering. The observed ESR line is interpreted as an Eu$^{2+}$ resonance, which probes the weak magnetic background of the Mn subsystem. Such picture is suggested by the lineshape which keeps to be Lorentzian across the $47\,\rm K$ scale and by the ESR intensity which can be described by the same Curie-Weiss temperature above and below $47\,\rm K$. In the same temperature range anomalies were observed at $48.5\,\rm K$ and $51\,\rm K$ in the heat capacity data as well as a pronounced broadening of the NMR signal of the EuMn$_{2}$P$_{2}$ samples. In XMCD and XMLD measurements, this weak magnetic order could not be detected in the same temperature range which might be due to the small magnetic moment, with a potential $c$-component or frustration.

cond-mat.str-el↗

arXiv2024

Controlling 4f antiferromagnetic dynamics via itinerant electronic susceptibility

Optical manipulation of magnetism holds promise for future ultrafast spintronics, especially with lanthanides and their huge, localized 4f magnetic moments. These moments interact indirectly via the conduction electrons (RKKY exchange), influenced by interatomic orbital overlap, and the conduction electron susceptibility. Here, we study this influence in a series of 4f antiferromagnets, GdT2Si2 (T=Co, Rh, Ir), using ultrafast resonant X-ray diffraction. We observe a twofold increase in ultrafast angular momentum transfer between the materials, originating from modifications in the conduction electron susceptibility, as confirmed by first-principles calculations.

cond-mat.mtrl-sci↗

arXiv2024

Magnetism, heat capacity and electronic structure of EuCd$_2$P$_2$ in view of its colossal magnetoresistance

The mechanism of the peculiar transport properties around the magnetic ordering temperature of semiconducting antiferromagnetic EuCd$_2$P$_2$ is not yet understood. With a huge peak in the resistivity observed above the Néel temperature, $T_{\rm N}=10.6\,\rm K$, it exhibits a colossal magnetoresistance effect. Recent reports on observations of ferromagnetic contributions above $T_{\rm N}$ as well as metallic behavior below this temperature have motivated us to perform a comprehensive characterization of this material, including its resistivity, heat capacity, magnetic properties and electronic structure. Our transport measurements revealed quite different temperature dependence of resistivity with the maximum at $14\,\rm K$ instead of previously reported $18\,\rm K$. Low-field susceptibility data support the presence of static ferromagnetism above $T_{\rm N}$ and show a complex behavior of the material at small applied magnetic fields. Namely, signatures of reorientation of magnetic domains are observed up to $T=16\,\rm K$. Our magnetization measurements indicate a magnetocrystalline anisotropy which also leads to a preferred alignment of the magnetic clusters above $T_{\rm N}$. The momentum-resolved photoemission experiments at temperatures from $24\,\rm K$ down to $2.5\,\rm K$ indicate the permanent presence of a fundamental band gap without change of the electronic structure when going through $T_N$ that is in contradiction with previous results. We performed \textit{ab initio} band structure calculations which are in good agreement with the measured photoemission data when assuming an antiferromagnetic ground state. Calculations for the ferromagnetic phase show a much smaller bandgap, indicating the importance of possible ferromagnetic contributions for the explanation of the colossal magnetoresistance effect in the related EuZn$_2$P$_2$.

cond-mat.str-el↗

arXiv2023

Simulating high-pressure surface reactions with molecular beams

Using a reactive molecular beam with high kinetic energy ($E_{kin}$) it is possible to speed gas-surface reactions involving high activation barriers ($E_{act}$), which would require elevated pressures ($P_0$) if a random gas with a Maxwell-Boltzmann distribution is used. By simply computing the number of molecules that overcome the activation barrier in a random gas at $P_0$ and in a molecular beam at $E_{kin}$=$E_{act}$, we establish an $E_{kin}$-$P_0$ equivalence curve, through which we postulate that molecular beams are ideal tools to investigate gas-surface reactions that involve high activation energies. In particular, we foresee the use of molecular beams to simulate gas surface reactions within the industrial-range ($>$ 10 bar) using surface-sensitive Ultra-High Vacuum (UHV) techniques, such as X-ray photoemission spectroscopy (XPS). To test this idea, we revisit the oxidation of the Cu(111) surface combining O$_2$ molecular beams and XPS experiments. By tuning the kinetic energy of the O$_2$ beam in the range 0.24-1 eV we achieve the same sequence of surface oxides obtained in Ambient Pressure Photoemission (AP-XPS) experiments, in which the Cu(111) surface was exposed to a random O$_2$ gas up to 1 mbar. We observe the same surface oxidation kinetics as in the random gas, but with a much lower dose, close to the expected value derived from the equivalence curve.

cond-mat.mtrl-sci↗

arXiv2023

Colossal magnetoresistance in EuZn$_2$P$_2$ and its electronic and magnetic structure

We investigate single crystals of the trigonal antiferromagnet EuZn$_2$P$_2$ ($P\overline{3}m1$) by means of electrical transport, magnetization measurements, X-ray magnetic scattering, optical reflectivity, angle-resolved photoemission spectroscopy (ARPES) and ab-initio band structure calculations (DFT+U). We find that the electrical resistivity of EuZn$_2$P$_2$ increases strongly upon cooling and can be suppressed in magnetic fields by several orders of magnitude (CMR effect). Resonant magnetic scattering reveals a magnetic ordering vector of $q = (0\, 0\, \frac{1}{2})$, corresponding to an $A$-type antiferromagnetic (AFM) order, below $T_{\rm N} = 23.7\,\rm K$. We find that the moments are canted out of the $a-a$ plane by an angle of about $40^{\circ}\pm 10^{\circ}$ degrees and aligned along the [100] in the $a-a$ plane. We observe nearly isotropic magnetization behavior for low fields and low temperatures which is consistent with the magnetic scattering results. The magnetization measurements show a deviation from the Curie-Weiss behavior below $\approx 150\,\rm K$, the temperature below which also the field dependence of the material's resistivity starts to increase. An analysis of the infrared reflectivity spectrum at $T=295\,\rm K$ allows us to resolve the main phonon bands and intra-/interband transitions, and estimate indirect and direct band gaps of $E_i^{\mathrm{opt}}=0.09\,\rm{eV}$ and $E_d^{\mathrm{opt}}=0.33\,\rm{eV}$, respectively, which are in good agreement with the theoretically predicted ones. The experimental band structure obtained by ARPES is nearly $T$-independent above and below $T_{\rm N}$. The comparison of the theoretical and experimental data shows a weak intermixing of the Eu 4$f$ states close to the $Γ$ point with the bands formed by the phosphorous 3$p$ orbitals leading to an induction of a small magnetic moment at the P sites.

cond-mat.str-el↗

arXiv2023

Moment canting and domain effects in antiferromagnetic DyRh$_2$Si$_2$

A combined experimental and theoretical study of the layered antiferromagnetic compound DyRh$_2$Si$_2$ in the ThCr$_2$Si$_2$-type structure is presented. The heat capacity shows two transitions upon cooling, the first one at the N{é}el temperature $T_{\rm N}=55\,\rm K$ and a second one at $T_{\rm N2}=12\,\rm K$. Using magnetization measurements, we study the canting process of the Dy moments upon changing the temperature and can assign $T_{\rm N2}$ to the onset of the canting of the magnetic moments towards the $[100]$ direction away from the $c$ axis. Furthermore, we found that the field dependence of the magnetization is highly anisotropic and shows a two-step process for $H\parallel 001$. We used a mean-field model to determine the crystalline electric field as well as the exchange interaction parameters. Our magnetization data together with the calculations reveal a moment orientation close to the $[101]$ direction in the tetragonal structure at low temperatures and fields. Applying photoemission electron microscopy, we explore the (001) surface of the cleaved DyRh$_2$Si$_2$ single crystal and visualize Si- and Dy-terminated surfaces. Our results indicate that the Si-Rh-Si surface protects the deeper lying magnetically active Dy layers and is thus attractive for investigation of magnetic domains and their properties in the large family of LnT$_2$Si$_2$ materials.

cond-mat.str-el↗

arXiv2022

Revealing intrinsic superconductivity of the Nb/BiSbTe$_2$Se interface

Typically, topological superconductivity is reachable via proximity effect by a direct deposition of superconductor (S) on top of a topological insulator (TI) surface. Here we observed and analyzed the double critical current in the Josephson junctions based on the topological insulator in the fabricated planar Superconducting Quantum Interference Device. By measuring critical currents as a function of temperature and magnetic field, we show that the second critical current stems from the intrinsic superconductivity of the S/TI interface, which is supported by the modified Resistively Shunted Junction model and Transmission Electron Microscopy studies. This complex structure of the interface should be taken into account when technological process involves Ar-plasma cleaning.

cond-mat.supr-con↗

arXiv2022

Robust magnetic order upon ultrafast excitation of an antiferromagnet

The ultrafast manipulation of magnetic order due to optical excitation is governed by the intricate flow of energy and momentum between the electron, lattice and spin subsystems. While various models are commonly employed to describe these dynamics, a prominent example being the microscopic three temperature model (M3TM), systematic, quantitative comparisons to both the dynamics of energy flow and magnetic order are scarce. Here, we apply a M3TM to the ultrafast magnetic order dynamics of the layered antiferromagnet GdRh$_2$Si$_2$. The femtosecond dynamics of electronic temperature, surface ferromagnetic order, and bulk antiferromagnetic order were explored at various pump fluences employing time- and angle-resolved photoemission spectroscopy and time-resolved resonant magnetic soft x-ray diffraction, respectively. After optical excitation, both the surface ferromagnetic order and the bulk antiferromagnetic order dynamics exhibit two-step demagnetization behaviors with two similar timescales (<1 ps, ~10 ps), indicating a strong exchange coupling between localized 4f and itinerant conduction electrons. Despite a good qualitative agreement, the M3TM predicts larger demagnetization than our experimental observation, which can be phenomenologically described by a transient, fluence-dependent increased Néel temperature. Our results indicate that effects beyond a mean-field description have to be considered for a quantitative description of ultrafast magnetic order dynamics.

cond-mat.str-el↗

arXiv2009

Dynamics of graphene growth on a metal surface: a time-dependent photoemission study

Applying time-dependent photoemission we unravel the graphene growth process on a metallic surface by chemical vapor deposition (CVD). Graphene CVD growth is in stark contrast to the standard growth process of two--dimensional films because it is self-limiting and stops as soon as a monolayer graphene has been synthesized. Most importantly, a novel phase of metastable graphene was discovered that is characterized by permanent and simultaneous construction and deconstruction. The high quality and large area graphene flakes are characterized by angle-resolved photoemission proofing that they are indeed monolayer and cover the whole 1$\times$1 cm Nickel substrate. These findings are of high relevance to the intensive search for reliable synthesis methods for large graphene flakes of controlled layer number.

cond-mat.mtrl-sci↗