arXiv subjects

Alexander N. Rudenko

Publications and source records attributed to Alexander N. Rudenko.

At least 19 recordsLinked to original sources

arXiv2024

Orbital-Selective Diffuse Magnetic Fluctuations in Sr$_2$RuO$_4$: a Unified Theoretical Picture

The quasi-two-dimensional material Sr$_2$RuO$_4$ is a paradigmatic example of a correlated system that exhibits unconventional superconductivity and intriguing magnetic properties. The interplay between these two effects and the resulting strength and nature of spin fluctuations and their role for the properties of the compound have sparked significant debates. Here, elaborating a theory that self-consistently incorporates spatial magnetic fluctuations into a realistic many-body description, we show that these fluctuations significantly reduce many-body correlations in the system, thereby preventing magnetic ordering in Sr$_2$RuO$_4$, in agreement with experimental observations. Our conclusion is supported by a theoretical calculation of the spin susceptibility that closely matches the experimental results. We obtain finite peaks at the incommensurate wave vectors, a broad dome-shaped structure centered around the $\Gamma$ point and a diminished magnetic response at the edges of the BZ. We identify the orbital character of the unusual dome structure as resulting predominantly from the 2D-like $xy$-orbital, which is believed to be responsible for the superconductivity.

cond-mat.str-el↗

arXiv2024

Realization of a one-dimensional topological insulator in ultrathin germanene nanoribbons

Realizing a one-dimensional (1D) topological insulator and identifying the lower dimensional limit of two-dimensional (2D) behavior are crucial steps toward developing high-density quantum state networks, advancing topological quantum computing, and exploring dimensionality effects in topological materials. Although 2D topological insulators have been experimentally realized, their lower dimensional limit and 1D counterparts remain elusive. Here, we fabricated and characterized arrays of zigzag-terminated germanene nanoribbons, a 2D topological insulator with a large topological bulk gap. The electronic properties of these nanoribbons strongly depend on their width, with topological edge states persisting down to a critical width (approx. 2 nm), defining the limit of 2D topology. Below this threshold, contrary to the tenfold way classification, we observe zero-dimensional (0D) states localized at the ends of the ultrathin nanoribbons. These end states, topologically protected by time-reversal and mirror symmetries, mark the first realization of a 1D topological insulator with strong spin-orbit coupling. Our findings establish germanene nanoribbons as a platform for investigating 1D topology and dimensionality effects in topological materials.

cond-mat.mes-hall↗

arXiv2024

Anisotropic effects in two-dimensional materials

Among a huge variety of known two-dimensional materials, some of them have anisotropic crystal structures; examples include so different systems as a few-layer black phoshphorus (phosphorene), beryllium nitride BeN$_4$, van der Waals magnet CrSBr, rhenium dichalgogenides ReX$_2$. As a consequence, their optical and electronic properties turn out to be highly anisotropic as well. In some cases, the anisotropy results not just in a smooth renormalization of observable properties in comparison with the isotropic case but in the appearance of dramatically new physics. The examples are hyperbolic plasmons and excitons, strongly anisotropic ordering of adatoms at the surface of two-dimensional or van der Waals materials, essential change of transport and superconducting properties. Here, we present a systematic review of electronic structure, transport and optical properties of several representative groups of anisotropic two-dimensional materials including semiconductors, anisotropic Dirac and semi-Dirac materials, as well as superconductors.

cond-mat.mtrl-sci↗

arXiv2024

Electrostatic Control of Magneto-Optic Excitonic Resonances in the van der Waals Ferromagnetic Semiconductor Cr$_2$Ge$_2$Te$_6$

Two-dimensional magnetic materials exhibit strong magneto-optic effects and high tunability by electrostatic gating, making them very attractive for new magneto-photonic devices. Here, we characterize the magneto-optic Kerr effect (MOKE) spectrum of thin Cr$_2$Ge$_2$Te$_6$ from 1.13 to 2.67 eV, and demonstrate electrostatic control over of its magnetic and magneto-optic properties. The MOKE spectrum exhibits a strong feature around 1.43 eV which we attribute to a magnetic exchange-split excitonic state in Cr$_2$Ge$_2$Te$_6$, in agreement with \textit{ab-initio} calculations. The gate dependence of the MOKE signals shows that the magneto-optical efficiency - rather than the saturation magnetization - is affected by electrostatic gating. We demonstrate a modulation of the magneto-optical strength by over 1 mdeg, with some wavelengths showing a modulation of 65% of the total magneto-optical signals, opening the door for efficient electrical control over light polarization through two-dimensional magnets. Our findings bring forward the fundamental understanding of magneto-optic processes in two-dimensional magnets and are highly relevant for the engineering of devices which exploit excitonic resonances for electrically-tunable magneto-photonic devices.

cond-mat.mes-hall↗

arXiv2024

Phonon-induced renormalization of exchange interactions in metallic two-dimensional magnets

The presence of spin-polarized charge carriers in metallic magnets provides a mechanism for spin-lattice interactions mediated by electron-phonon coupling. Here, we present a theory of this mechanism used to estimate its effect on the exchange interactions in 2D magnets. Starting from a square lattice model at half filling, we show that the presence of electron-phonon coupling with equilibrium phonon distribution leads to a notable suppression of exchange interactions with temperature. We then apply our approach to the prototypical 2D metallic ferromagnet, Fe$_3$GeTe$_2$, with moderate electron-phonon coupling. We find that the exchange interactions undergo a renormalization, leading to a softening of the magnon modes, and suppression of the Curie temperature by $\sim$10\%. We expect that this effect can be further enhanced in systems with strong electron-phonon coupling, as well as for non-equilibrium distribution of phonons induced by strong laser fields or charge currents.

cond-mat.mtrl-sci↗

arXiv2024

Strong electron-phonon coupling and phonon-induced superconductivity in tetragonal C$_3$N$_4$ with hole doping

C$_3$N$_4$ is a recently discovered phase of carbon nitrides with the tetragonal crystal structure [D.Laniel $\textit{et al.}$, Adv. Mater. 2023, 2308030] that is stable at ambient conditions. C$_3$N$_4$ is a semiconductor exhibiting flat-band anomalies in the valence band, suggesting the emergence of many-body instabilities upon hole doping. Here, using state-of-the-art first-principles calculations we show that hole-doped C$_3$N$_4$ reveals strong electron-phonon coupling, leading to the formation of a gapped superconducting state. The phase transition temperatures turn out to be strongly dependent on the hole concentration. We propose that holes could be injected into C$_3$N$_4$ via boron doping which induces, according to our results, a rigid shift of the Fermi energy without significant modification of the electronic structure. Based on the electron-phonon coupling and Coulomb pseudopotential calculated from first principles, we conclude that the boron concentration of 6 atoms per nm$^3$ would be required to reach the critical temperature of $\sim$36 K at ambient pressure.

cond-mat.supr-con↗

arXiv2023

An effective spin model on the honeycomb lattice for the description of magnetic properties in two-dimensional Fe$_3$GeTe$_2$

Fe$_3$GeTe$_2$ attracts significant attention due to technological perspectives of realizing room temperature ferromagnetism in two-dimensional materials. Here we show that due to structural peculiarities of the Fe$_3$GeTe$_2$ monolayer, short distance between the neighboring iron atoms induces a strong exchange coupling. This strong coupling allows us to consider them as an effective cluster with a magnetic moment $\sim$5 $μ_B$, giving rise to a simplified spin model on a bipartite honeycomb lattice with the reduced number of long-range interactions. The simplified model perfectly reproduces the results of the conventional spin model, but allows for a more tractable description of the magnetic properties of Fe$_3$GeTe$_2$, which is important, e.g., for large-scale simulations. Also, we discuss the role of biaxial strain in the stabilization of ferromagnetic ordering in Fe$_3$GeTe$_2$.

cond-mat.mtrl-sci↗

arXiv2023

Charge transfer-induced Lifshitz transition and magnetic symmetry breaking in ultrathin CrSBr crystals

Ultrathin CrSBr flakes are exfoliated \emph{in situ} on Au(111) and Ag(111) and their electronic structure is studied by angle-resolved photoemission spectroscopy. The thin flakes' electronic properties are drastically different from those of the bulk material and also substrate-dependent. For both substrates, a strong charge transfer to the flakes is observed, partly populating the conduction band and giving rise to a highly anisotropic Fermi contour with an Ohmic contact to the substrate. The fundamental CrSBr band gap is strongly renormalized compared to the bulk. The charge transfer to the CrSBr flake is substantially larger for Ag(111) than for Au(111), but a rigid energy shift of the chemical potential is insufficient to describe the observed band structure modifications. In particular, the Fermi contour shows a Lifshitz transition, the fundamental band gap undergoes a transition from direct on Au(111) to indirect on Ag(111) and a doping-induced symmetry breaking between the intra-layer Cr magnetic moments further modifies the band structure. Electronic structure calculations can account for non-rigid Lifshitz-type band structure changes in thin CrSBr as a function of doping and strain. In contrast to undoped bulk band structure calculations that require self-consistent $GW$ theory, the doped thin film properties are well-approximated by density functional theory if local Coulomb interactions are taken into account on the mean-field level and the charge transfer is considered.

cond-mat.str-el↗

arXiv2023

Paramagnetic Electronic Structure of CrSBr: Comparison between Ab Initio GW Theory and Angle-Resolved Photoemission Spectroscopy

We explore the electronic structure of paramagnetic CrSBr by comparative first principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent $GW$ theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QS$GW$ and QS$G\hat{W}$, respectively). Comparing the quasi-particle band structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of $\approx$ 2.1 eV.

cond-mat.str-el↗

arXiv2023

Dielectric tunability of magnetic properties in orthorhombic ferromagnetic monolayer CrSBr

Monolayer CrSBr is a recently discovered semiconducting spin-3/2 ferromagnet with a Curie temperature around 146 K. Unlike many other known two-dimensional (2D) magnets, CrSBr has an orthorhombic lattice, giving rise, for instance, to spatial anisotropy of the magnetic excitations within the 2D plane. Theoretical description of CrSBr within a spin Hamiltonian approach turns out to be nontrivial due to the triaxial magnetic anisotropy as well as due to magnetic dipolar interactions, comparable to spin-orbit effects in CrSBr. Here, we employ a Green's function formalism combined with first-principles calculations to systematically study the magnetic properties of monolayer CrSBr in different regimes of surrounding dielectric screening. We find that the magnetic anisotropy and thermodynamical properties of CrSBr depend significantly on the Coulomb interaction and its external screening. In the free-standing limit, the system turns out to be close to an easy-plane magnet, whose long-range ordering is partially suppressed. On the contrary, in the regime of large external screening, monolayer CrSBr behaves like an easy-axis ferromagnet with more stable magnetic ordering. Despite being relatively large, the magnetic dipolar interactions have only little effect on the magnetic properties. Our findings suggests that 2D CrSBr is suitable platform for studying the effects of substrate screening on magnetic ordering in low dimensions.

cond-mat.mtrl-sci↗

arXiv2023

Electron transport and scattering mechanisms in ferromagnetic monolayer Fe$_3$GeTe$_2$

We study intrinsic charge-carrier scattering mechanisms and determine their contribution to the transport properties of the two-dimensional ferromagnet Fe$_3$GeTe$_2$. We use state-of-the-art first-principles calculations combined with the model approaches to elucidate the role of the electron-phonon and electron-magnon interactions in the electronic transport. Our findings show that the charge carrier scattering in Fe$_3$GeTe$_2$ is dominated by the electron-phonon interaction, while the role of magnetic excitations is marginal. At the same time, the magnetic ordering is shown to effect essentially on the electron-phonon coupling and its temperature dependence. This leads to a sublinear temperature dependence of the electrical resistivity near the Curie temperature, which is in line with experimental observations. The room temperature resistivity is estimated to be $\sim$35 $μΩ\cdot$cm which may be considered as an intrinsic limit for monolayer Fe$_3$GeTe$_2$.

cond-mat.mtrl-sci↗

arXiv2022

Electronic and optical properties of crystalline nitrogen versus black phosphorus: A comparative first-principles study

Crystalline black nitrogen (BN) is an allotrope of nitrogen with the black phosphorus (BP) structure recently synthesized at high pressure by two independent research groups [Ji et al., Sci. Adv. 6, eaba9206 (2020); Laniel et al., Phys. Rev. Lett. 124, 216001 (2020)]. Here, we present a systematic study of the electronic and optical properties of BN focusing on its comparison with BP. To this end, we use the state-of-the-art quasiparticle self-consistent $GW$ approach with vertex corrections in both the electronic and optical channels. Despite many similarities, the properties of BN are found to be considerably different. Unlike BP, BN exhibits a larger optical gap (2.5 vs 0.26 eV), making BN transparent in the visible spectral region with a highly anisotropic optical response. This difference can be primarily attributed to a considerably reduced dielectric screening in BN, leading to enhancement of the effective Coulomb interaction. Despite relatively strong Coulomb interaction, exciton formation is largely suppressed in both materials. Our analysis of the elastic properties shows exceptionally high stiffness of BN, comparable to that of diamond.

cond-mat.mtrl-sci↗

arXiv2022

Dynamical correlations in single-layer CrI$_3$

Chromium triiodide is an intrinsically magnetic van der Waals material down to the single-layer limit. Here, we provide a first-principles description of finite-temperature magnetic and spectral properties of monolayer (ML) CrI$_3$ based on fully charge self-consistent density functional theory (DFT) combined with dynamical mean-field theory, revealing a formation of local moments on Cr from strong local Coulomb interactions. We show that the presence of local dynamical correlations leads to a modification of the electronic structure of ferromagnetically ordered CrI$_3$. In contrast to conventional DFT+$U$ calculations, we find that the top of the valence band in ML CrI$_3$ demonstrates essentially different orbital character for minority and majority spin states, which is closer to the standard DFT results. This leads to a strong spin polarization of the optical conductivity upon hole doping, which could be verified experimentally.

cond-mat.str-el↗

arXiv2022

Orbital memory from individual Fe atoms on black phosphorus

Bistable valency in individual atoms presents a new approach toward single-atom memory, as well as a building block to create tunable and stochastic multi-well energy landscapes. Yet, this concept of orbital memory has thus far only been observed for cobalt atoms on the surface of black phosphorus, which are switched using tip-induced ionization. Here, we show that individual iron atoms on the surface of black phosphorus exhibit orbital memory using a combination of scanning tunneling microscopy and spectroscopy with ab initio calculations based on density functional theory. Unlike cobalt, the iron orbital memory can be switched in its non-ionized ground state. Based on calculations, we confirm that each iron valency has a distinct magnetic moment that is characterized by a distinguishable charge distribution due to the different orbital population. By studying the stochastic switching of the valency with varying tunneling conditions, we propose that the switching mechanism is based on a two-electron tunneling process.

cond-mat.mes-hall↗

arXiv2022

Gating orbital memory with an atomic donor

Orbital memory is defined by two stable valencies that can be electrically switched and read-out. To explore the influence of an electric field on orbital memory, we studied the distance-dependent influence of an atomic Cu donor on the state favorability of an individual Co atom on black phosphorus. Using low temperature scanning tunneling microscopy/spectroscopy, we characterized the electronic properties of individual Cu donors, corroborating this behavior with ab initio calculations based on density functional theory. We studied the influence of an individual donor on the charging energy and stochastic behavior of an individual Co atom. We found a strong impact on the state favorability in the stochastic limit. These findings provide quantitative information about the influence of local electric fields on atomic orbital memory.

cond-mat.mes-hall↗

arXiv2021

Excitons in Bulk and Layered Chromium Tri-Halides: From Frenkel to the Wannier-Mott Limit

Excitons with large binding energies $\sim$2-3 eV in CrX$_{3}$ are historically characterized as being localized (Frenkel) excitons that emerge from the atomic $d{-}d$ transitions between the Cr-3$d$-$t_{2g}$ and $e_{g}$ orbitals. The argument has gathered strength in recent years as the excitons in recently made monolayers are found at almost the same energies as the bulk. The Laporte rule, which restricts such parity forbidden atomic transitions, can relax if, at least, one element is present: spin-orbit coupling, odd-parity phonons or Jahn-Teller distortion. While what can be classified as a purely Frenkel exciton is a matter of definition, we show using an advanced first principles parameter-free approach that these excitons in CrX$_{3}$, in both its bulk and monolayer variants, have band-origin and do not require the relaxation of Laporte rule as a fundamental principle. We show that, the character of these excitons is mostly determined by the Cr-$d$ orbital manifold, nevertheless, they appear only as a consequence of X-p states hybridizing with the Cr-$d$. The hybridization enhances as the halogen atom becomes heavier, bringing the X-$p$ states closer to the Cr-$d$ states in the sequence Cl{\textrightarrow}Br{\textrightarrow}I, with an attendant increase in exciton intensity and decrease in binding energy. By applying a range of different kinds of perturbations, we show that, moderate changes to the two-particle Hamiltonian that essentially modifies the Cr-$d$-X-$p$ hybridization, can alter both the intensities and positions of the exciton peaks. A detailed analysis of several deep lying excitons, with and without strain, reveals that the exciton is most Frenkel like in CrCl$_{3}$ and acquires mixed Frenkel-Wannier character in CrI$_{3}$.

cond-mat.mtrl-sci↗

arXiv2021

First principles vs second principles: Role of charge self-consistency in strongly correlated systems

First principles approaches have been successful in solving many-body Hamiltonians for real materials to an extent when correlations are weak or moderate. As the electronic correlations become stronger often embedding methods based on first principles approaches are used to better treat the correlations by solving a suitably chosen many-body Hamiltonian with a higher level theory. Such combined methods are often referred to as second principles approaches. At such level of the theory the self energy, i.e. the functional that embodies the stronger electronic correlations, is either a function of energy or momentum or both. The success of such theories is commonly measured by the quality of the self energy functional. However, self-consistency in the self-energy should, in principle, also change the real space charge distribution in a correlated material and be able to modify the electronic eigenfunctions, which is often undermined in second principles approaches. Here we study the impact of charge self-consistency within two example cases: TiSe$_{2}$, a three-dimensional charge-density-wave candidate material, and CrBr$_{3}$, a two-dimensional ferromagnet, and show how real space charge re-distribution due to correlation effects taken into account within a first principles Green's function based many-body perturbative approach is key in driving qualitative changes to the final electronic structure of these materials.

cond-mat.str-el↗

arXiv2021

Electronic Structure of Chromium Trihalides beyond Density Functional Theory

We explore the electronic band structure of free standing monolayers of chromium trihalides, CrX\textsubscript{3}{, X= Cl, Br, I}, within an advanced \emph{ab-initio} theoretical approach based in the use of Green's function functionals. We compare the local density approximation with the quasi-particle self-consistent \emph{GW} approximation (QS\emph{GW}) and its self-consistent extension (QS$G\widehat{W}$) by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction \emph{W}. We show that at all levels of theory, the valence band consistently changes shape in the sequence Cl{\textrightarrow}Br{\textrightarrow}I, and the valence band maximum shifts from the M point to the $Γ$ point. However, the details of the transition, the one-particle bandgap, and the eigenfunctions change considerably going up the ladder to higher levels of theory. The eigenfunctions become more directional, and at the M point there is a strong anisotropy in the effective mass. Also the dynamic and momentum dependent self energy shows that QS$G\widehat{W}$ adds to the localization of the systems in comparison to the QS\emph{GW} thereby leading to a narrower band and reduced amount of halogens in the valence band manifold.

cond-mat.str-el↗