arXiv subjects

Irina V. Lebedeva

Publications and source records attributed to Irina V. Lebedeva.

At least 19 recordsLinked to original sources

arXiv2026

Taming quantum interference: a route to high electrical conductance in carbon nanotube assemblies

In nanostructured networks, transport is governed by junctions between neighbouring building blocks. Improving their alignment and removing defects is the intuitive route to better electron transport. At low temperatures, when transport becomes coherent, a junction cannot always be reduced to a single effective resistance, because electron-wave interference can strongly enhance or suppress transmission even in nominally ideal junctions. Using carbon nanotube (CNT) networks as a model system, we explore coherent transport through experimentally relevant junctions, from single and multiple single-walled CNT (SWCNT) contacts to double-walled CNT (DWCNT) and multi-walled CNT (MWCNT) junctions, with atomistic tight-binding non-equilibrium Green's-function calculations, also under a perpendicular magnetic field. We use analytically solvable minimal models to identify transport regimes expected for quasi-1D nanoscale junctions, and an electron-waveguide picture to interpret their CNT-specific manifestations. For single SWCNT--SWCNT junctions, high-transmission windows are set mainly by overlap length, doping and magnetic field. Gateway states can enhance conductance when some CNT subbands are gapped, and in some cases a magnetic field can restore transmission by lifting an interference blockade. In more complex architectures, added paths become selective: multi-junctions generate resonant filtering, while additional walls redistribute transmission instead of acting as independent channels. DWCNT junctions remain outer-wall dominated and SWCNT-like, whereas MWCNT junctions redistribute transmission among coupled walls and show a more complex field response. Our ultrahigh-field measurements likewise show lower, more field-sensitive conductance in MWCNT than SWCNT fibres. This work turns microscopic interference mechanisms into design principles for high-conductance, field-stable CNT conductors.

cond-mat.mes-hall↗

arXiv2025

Robust structural superlubricity of twisted graphene bilayer and domain walls between commensurate moiré pattern domains from first-principles calculations

Twisted graphene layers exhibit extremely low friction for relative sliding. Nevertheless, previous studies suggest that the area contribution to friction for commensurate moiré systems is finite and might restrict macroscopic superlubricity for large layer overlaps. In this paper, we investigate the potential energy surface (PES) for relative displacement of the layers forming moiré patterns (2,1) and (3,1) by accurate density functional theory calculations using the vdW-DF3 functional. The amplitudes of PES corrugations on the order of 0.4 and 0.03 $μ$eV per atom of one layer, respectively, are obtained. The account of structural relaxation doubles this value for the (2,1) pattern, while causing only minimal changes for the (3,1) pattern. We show that different from aligned graphene layers, for moiré patterns, PES minima and maxima can switch their positions upon changing the interlayer distance. The PES shape is closely described by the first spatial Fourier harmonics both with and without account of structural relaxation. A barrier for relative rotation of the layers to an incommensurate state that can make superlubricity robust is estimated based on the approximated PES. We also derive a set of measurable physical properties related to interlayer interaction including shear mode frequency, shear modulus and static friction force. Furthermore, we predict that it should be possible to observe domain walls separating commensurate domains, each comprising a large number of moiré pattern unit cells, and provide estimates of their characteristics.

cond-mat.mes-hall↗

arXiv2025

Restriction of macroscopic structural superlubricity due to structure relaxation by the example of twisted graphene bilayer

The effect of structure relaxation on the potential energy surface (PES) of interlayer interaction of twisted graphene bilayer is studied for a set of commensurate moiré systems using the registry-dependent empirical potential of Kolmogorov and Crespi. It is found that the influence of structure relaxation on the amplitude of PES corrugations (determining static friction) depends on the unit cell size (or related twist angle) of the moiré system. For moiré systems with the smallest unit cells, the amplitudes of PES corrugations calculated with and without account of structure relaxation are approximately the same. However, for large unit cell sizes, the structure relaxation can lead to an increase of PES corrugations by orders of magnitude. This means that structure relaxation can provide the main contribution into the static friction of a superlubric system under certain conditions (such as the contact size and twist angle). Moreover, the change of the PES type because of structure relaxation from a trigonal lattice of maxima to a trigonal lattice of minima is observed for the systems with the moiré patterns (5,1) and (5,3). Based on the results obtained, possible crossovers between static friction modes taking place upon changing the twist angle in a macroscopic superlubric system consisting of identical layers are discussed. Additionally it is shown that the PES for relaxed structures can still be approximated by the first Fourier harmonics compatible with symmetries of twisted layers analogously to the PES for rigid layers.

cond-mat.mes-hall↗

arXiv2024

Magnetic and electronic properties of 1D hybrid nanoobjects composed of alternating polycyclic hydrocarbon regions and double carbon chains

It has been proposed recently that 1D hybrid nanoobjects consisting of alternating double carbon chains and polycyclic carbon regions can be obtained from graphene nanoribbons of alternating width by electron irradiation. Here, based on density functional theory calculations, we show that magnetic and electronic properties of such nanoobjects can be changed dramatically by modifying the chain length and edge structure of polycyclic regions and this opens wide possibilities for spintronic applications. Nanoobjects composed of polycyclic regions with dangling bonds and even chains are found to behave as magnetic semiconductors that can generate spin-polarized currents. Band gaps of nanoobjects with odd chains change considerably upon switching between magnetic states making them promising for magnetic tunnel junctions. We also demonstrate that use of a hybrid exchange-correlation functional is important to properly describe stability of magnetic states, band gaps and synergistic effects of nanoobject components leading, for example, to magnetism in even chains.

cond-mat.mes-hall↗

arXiv2024

Optical properties and exciton transfer between N-heterocyclic carbene iridium (III) complexes for blue light-emitting diode applications from first principles

N-heterocyclic carbene (NHC) iridium (III) complexes are considered as promising candidates for blue emitters in organic light-emitting diodes. They can play the roles of the emitter as well as of electron and hole transporters in the same emission layer. We investigate optical transitions in such complexes with account of geometry and electronic structure changes upon excitation or charging and exciton transfer between the complexes from first principles. It is shown that excitation of NHC iridium complexes is accompanied by a large reorganization energy $\sim$0.7 eV and a significant loss in the oscillator strength, which should lead to low exciton diffusion. Calculations with account of spin-orbit coupling reveal a small singlet-triplet splitting $\sim$0.1 eV, whereas the oscillator strength for triplet excitations is found to be an order of magnitude smaller than for the singlet ones. The contributions of the Förster and Dexter mechanisms are analyzed via the explicit integration of transition densities. It is shown that for typical distances between emitter complexes in the emission layer, the contribution of the Dexter mechanism should be negligible compared to the Förster mechanism. On the other hand, the ideal dipole approximation, although gives the correct order of the exciton coupling, fails to reproduce the result taking into account spatial distribution of the transition density. For charged NHC complexes, we find a number of optical transitions close to the emission peak of the blue emitter with high exciton transfer rates that can be responsible for exciton-polaron quenching. The nature of these transitions is analyzed.

cond-mat.mtrl-sci↗

arXiv2023

Interlayer interaction, shear vibrational mode, and tribological properties of two-dimensional bilayers with a commensurate moiré pattern

The potential energy surface (PES) of interlayer interaction of infinite twisted bilayer graphene is calculated for a set of commensurate moiré patterns using the registry-dependent Kolmogorov-Crespi empirical potential. The calculated PESs have the same shape for all considered moiré patterns with the unit cell size of the PES which is inversely related to the unit cell size of the moiré pattern. The amplitude of PES corrugations is found to decrease exponentially upon increasing the size of the moiré pattern unit cell. An analytical expression for such a PES including the first Fourier harmonics compatible with the symmetries of both layers is derived. It is shown that the calculated PESs can be approximated by the derived expression with the accuracy within 1%. This means that different physical properties associated with relative in-plane motion of graphene layers are interrelated and can be expressed analytically as functions of the amplitude of PES corrugations. In this way, we obtain the shear mode frequency, shear modulus, shear strength and barrier for relative rotation of the commensurate twisted layers to a fully incommensurate state for the considered moiré patterns. This barrier may possibly lead to the macroscopic robust superlubricity for twisted graphene bilayer with a commensurate moiré pattern. The conclusions made should be valid for diverse 2D systems of twisted commensurate layers.

cond-mat.mes-hall↗

arXiv2023

Modular implementation of the linear and cubic-scaling orbital minimization methods in electronic structure codes using atomic orbitals

We present a code modularization approach to design efficient and massively parallel cubic and linear-scaling solvers for electronic structure calculations using atomic orbitals. The modular implementation of the orbital minimization method, in which linear algebra and parallelization issues are handled via external libraries, is demonstrated in the SIESTA code. The DBCSR and ScaLAPACK libraries are used for algebraic operations with sparse and dense matrices, respectively. The MatrixSwitch and libOMM libraries, recently developed within the Electronic Structure Library, facilitate switching between different matrix formats and implement the energy minimization. We show results comparing the performance of several cubic-scaling algorithms, and also demonstrate the parallel performance of the linear-scaling solvers, and their supremacy over the cubic-scaling solvers for insulating systems with sizes of several hundreds of atoms.

cond-mat.mtrl-sci↗

arXiv2022

Optimal model of semi-infinite graphene for ab initio calculations of reactions at graphene edges by the example of zigzag edge reconstruction

We investigate how parameters of the model of semi-infinite graphene based on a graphene nanoribbon under periodic boundary conditions affect the accuracy of ab initio calculations of reactions at graphene edges by the example of the first stage of reconstruction of zigzag graphene edges, formation of a pentagon-heptagon pair. It is shown that to converge properly the results, the nanoribbon should consist of at least 6 zigzag rows and periodic images of the pair along the nanoribbon axis should be separated by at least 6 hexagons. The converged reaction energy and activation barrier for formation of an isolated pentagon-heptagon pair are found to be -0.15 eV and 1.61 eV, respectively. It is also revealed that such defects reduce the graphene edge magnetization only locally but ordering of spins at opposite nanoribbon edges switches from the antiparallel (antiferromagnetic) to parallel one (ferromagnetic) upon increasing the defect density.

cond-mat.mes-hall↗

arXiv2022

Reconstruction of Zigzag Graphene Edges: Energetics, Kinetics and Residual Defects

Ab initio calculations are performed to study consecutive reconstruction of a zigzag graphene edge. According to the obtained energy profile along the reaction pathway, the first reconstruction step, formation of the first pentagon-heptagon pair, is the slowest one, while the growth of an already nucleated reconstructed edge domain should occur steadily at a much higher rate. Domains merge into one only in 1/4 of cases when they get in contact, while in the rest of the cases, residual defects are left. Structure, energy and magnetic properties of these defects are studied. It is found that spontaneous formation of pairs of residual defects (i.e. spontaneous domain nucleation) in the fully reconstructed edge is unlikely at temperatures below 1000 K. Using a kinetic model, we show that the average domain length is of several $\mathrmμ$m at room temperature and it decreases exponentially upon increasing the temperature at which the reconstruction takes place.

cond-mat.mes-hall↗

arXiv2021

Atomic-scale defects restricting structural superlubricity: Ab initio study study on the example of the twisted graphene bilayer

The potential energy surface (PES) of interlayer interaction of twisted bilayer graphene with vacancies in one of the layers is investigated via density functional theory (DFT) calculations with van der Waals corrections. These calculations give a non-negligible magnitude of PES corrugation of 28 meV per vacancy and barriers for relative sliding of the layers of 7 - 8 meV per vacancy for the moiré pattern with coprime indices (2,1) (twist angle 21.8$^\circ$). At the same time, using the semiempirical potential fitted to the DFT results, we confirm that twisted bilayer graphene without defects exhibits superlubricity for the same moiré pattern and the magnitude of PES corrugation for the infinite bilayer is below the calculation accuracy. Our results imply that atomic-scale defects restrict the superlubricity of 2D layers and can determine static and dynamic tribological properties of these layers in a superlubric state. We also analyze computationally cheap approaches that can be used for modeling of tribological behavior of large-scale systems with defects. The adequacy of using state-of-the-art semiempirical potentials for interlayer interaction and approximations based on the first spatial Fourier harmonics for the description of interaction between graphene layers with defects is discussed.

cond-mat.mes-hall↗

arXiv2021

Multiscale modeling strategy to solve fullerene formation mystery

Since fullerene formation occurs under conditions where direct observation of atomic-scale reactions is not possible, modeling is the only way to reveal atomistic mechanisms which can lead to selection of abundant fullerene isomers (like C60-Ih). In the present paper we review the results obtained for different atomistic mechanisms by various modeling techniques. Although it seems that atomic-scale processes related to odd fullerenes (such as growth by consecutive insertions of single carbon atoms and rearrangements of the sp$^2$ structure promoted by extra sp atoms) provide the main contribution to selection of abundant isomers, at the moment there is no conclusive evidence in favor of any particular atomistic mechanism. Thus, the following multiscale modeling strategy to solve the mystery of the high yield of abundant fullerene isomers is suggested. On the one hand, sets of reactions between fullerene isomers can be described using theoretical graph techniques. On the other hand, reaction schemes can be revealed by classical molecular dynamics simulations with subsequent refinement of the activation barriers by ab initio calculations. Based on the reaction sets with the reaction probabilities derived in this way, the different atomistic mechanisms of abundant fullerene isomer selection can be compared by kinetic models.

cond-mat.mes-hall↗

arXiv2021

Healing of a hole in a carbon nanotube under electron irradiation in HRTEM

Healing of a hole in a carbon nanotube under electron irradiation in HRTEM at room temperature is demonstrated using molecular dynamics simulations with the CompuTEM algorithm. Formation of an amorphous patch is observed in all simulation runs. The amorphous patch is formed in the absence of external carbon adatoms only via reconstruction of the carbon bond network. It consists mainly of 5-, 6- and 7-membered rings and causes a small bottleneck. In addition, further growth of the initial amorphous patch under electron irradiation takes place. Two-coordinated atoms are found to play a crucial role in the latter process, analogous to autocatalisys of rearrangements of rings in fullerenes. The principal rearrangements in the presence of two-coordinated atoms can be described as generalized sp-defect migration: a bond is broken between two three-coordinated atoms and one of them forms a new bond with a nearby two-coordinated atom. If the new and former two-coordinated atoms are not bonded, the reaction leads both to displacement of the sp defect and changes in rings of the sp$^2$ carbon structure. Migration by hopping of two-coordinated atoms and other reactions involving simultaneous breakage of two bonds are also detected but much rarely. Long-living two-coordinated atoms in the patch structure and related fast growth of the patch are observed in more than half of the simulation runs. Since the amorphous patch and bottleneck affect the electronic properties of the nanotube, such nanotubes can be perspective for nanoelectronic applications.

cond-mat.mes-hall↗

arXiv2021

Transformation of a graphene nanoribbon into a hybrid 1D nanoobject with alternating double chains and polycyclic regions

Molecular dynamics simulations show that a graphene nanoribbon with alternating regions which are one and three hexagons wide can transform into a hybrid 1D nanoobject with alternating double chains and polycyclic regions under electron irradiation in HRTEM. A scheme of synthesis of such a nanoribbon using Ullmann coupling and dehydrogenation reactions is proposed. The reactive REBO-1990EVC potential is adapted for simulations of carbon-hydrogen systems and is used in combination with the CompuTEM algorithm for modeling of electron irradiation effects. The atomistic mechanism of formation of the new hybrid 1D nanoobject is found to be the following. Firstly hydrogen is removed by electron impacts. Then spontaneous breaking of bonds between carbon atoms leads to decomposition of narrow regions of the graphene nanoribbon into double chains. Simultaneously thermally activated growth of polycyclic regions occurs. Density functional theory calculations give barriers along the growth path of polycyclic regions consistent with this mechanism. Electronic properties of the new 1D nanoobject are shown to be strongly affected by the edge magnetism and make this nanostructure promising nanoelectronic and spintronic applications. The way of synthesis the 1D nanoobject proposed here can be considered as an example of the general three-stage strategy of production of nanoobjects and macromolecules. 1) precursors are synthesized by traditional chemical method, 2) precursors are placed in HRTEM with the electron energy that is sufficient only to remove hydrogen atoms, 3) as a result of hydrogen removal, the precursors become unstable or metastable and transform into new nanoobjects or macromolecules.

cond-mat.mes-hall↗

arXiv2020

Molecular Dynamics Study of sp-Defect Migration in Odd Fullerene: Possible Role in Synthesis of Abundant Isomers of Fullerenes

To explain recent experiment showing the role of odd fullerenes in formation of abundant fullerene isomers a reactive molecular dynamics (MD) study has been performed. Three types of bond rearrangement reactions are found by MD simulations at 3000 K in odd fullerenes which contain an extra sp atom among all other sp$^2$ atoms. The first type is sto-chastic sp-defect migration analogous to exchange mechanism of adatom migration on a surface. The second type cor-responds to changes in the ring configuration of the sp$^2$-structure assisted by the sp atom which can lead to annealing of seven-membered rings or separation of five-membered rings. The third type is formation of short-living one-coordinated atoms or two additional sp atoms. Annihilation of a pair of sp defects has been also observed in the MD simulations. It is shown that the frequency of sp-defect migration at a lower temperature, as estimated from performed density functional theory calculations of the barriers of sp-defect migration events, is sufficient to deliver the sp atom to defects of sp$^2$ structure during the fullerene formation time. Based on these results, we propose to supplement the self-organization paradigm of fullerene formation by the following four-stage atomistic mechanism of formation of abundant isomers of fullerenes: 1) attachment of single carbon atoms, 2) sp-defect migration to sp$^2$-structure defects, 3) sp$^2$-defect annealing assisted by the sp atom and 4) subsequent annihilation of pairs of sp defects.

cond-mat.mes-hall↗

arXiv2020

Universal description of potential energy surface of interlayer interaction in two-dimensional materials by first spatial Fourier harmonics

We propose a hypothesis that the potential energy surface (PES) of interlayer interaction in diverse 2D materials can be universally described by the first spatial Fourier harmonics. This statement (checked previously for the interactions between graphene and hexagonal boron nitride layers in different combinations) is verified in the present paper for the case of hydrofluorinated graphene (HFG) bilayer with hydrogen bonding between fluorine and hydrogen at the interlayer interface. The PES for HFG bilayer is obtained through density functional theory calculations with van der Waals corrections. An analytical expression based on the first Fourier harmonics describing the PES which corresponds to the symmetry of HFG layers is derived. It is found that the calculated PES can be described by the first Fourier harmonics with the accuracy of 3\% relative to the PES corrugation. The shear mode frequency, shear modulus and barrier for relative rotation of the layers to incommensurate states of HFG bilayer are estimated. Additionally it is shown that HFG bilayer is stable relative to the formation of HF molecules as a result of chemical reactions between the layers.

cond-mat.mes-hall↗

arXiv2020

The CECAM Electronic Structure Library and the modular software development paradigm

First-principles electronic structure calculations are very widely used thanks to the many successful software packages available. Their traditional coding paradigm is monolithic, i.e., regardless of how modular its internal structure may be, the code is built independently from others, from the compiler up, with the exception of linear-algebra and message-passing libraries. This model has been quite successful for decades. The rapid progress in methodology, however, has resulted in an ever increasing complexity of those programs, which implies a growing amount of replication in coding and in the recurrent re-engineering needed to adapt to evolving hardware architecture. The Electronic Structure Library (\esl) was initiated by CECAM (European Centre for Atomic and Molecular Calculations) to catalyze a paradigm shift away from the monolithic model and promote modularization, with the ambition to extract common tasks from electronic structure programs and redesign them as free, open-source libraries. They include "heavy-duty" ones with a high degree of parallelisation, and potential for adaptation to novel hardware within them, thereby separating the sophisticated computer science aspects of performance optimization and re-engineering from the computational science done by scientists when implementing new ideas. It is a community effort, undertaken by developers of various successful codes, now facing the challenges arising in the new model. This modular paradigm will improve overall coding efficiency and enable specialists (computer scientists or computational scientists) to use their skills more effectively. It will lead to a more sustainable and dynamic evolution of software as well as lower barriers to entry for new developers.

cond-mat.mtrl-sci↗

arXiv2020

Two phases with different domain wall networks and a reentrant phase transition in bilayer graphene under strain

The analytical two-chain Frenkel-Kontorova model is used to describe domain wall networks in bilayer graphene upon biaxial stretching of one of the layers. We show that the commensurate-incommensurate phase transition leading to formation of a regular triangular domain wall network at the relative biaxial elongation of $3.0\cdot 10^{-3}$ is followed by the transition to another incommensurate phase with a striped network at the elongation of $3.7\cdot 10^{-3}$. The reentrant transition to the phase with a triangular domain wall network is predicted for the elongation $\sim10^{-2}$.

cond-mat.mes-hall↗

arXiv2020

Energetics and Structure of Domain Wall Networks in Minimally Twisted Bilayer Graphene under Strain

The parameters of the triangular domain wall network in bilayer graphene with a simultaneously twisted and biaxially stretched bottom layer are studied using the two-chain Frenkel-Kontorova model. It is demonstrated that if the graphene layers are free to rotate, they prefer to stay co-aligned upon stretching the bottom layer and the regular triangular network of tensile domain walls is formed upon the commensurate-incommensurate phase transition. If the angle between the layers is fixed, the regular triangular network of shear domain walls is observed at zero elongation of the bottom layer. Upon stretching the bottom layer, however, the domain walls transform into the tensile ones and the size of the commensurate domains decreases. We also show that the parameters of the isosceles triangular domain wall network in twisted bilayer graphene under shear strain can be determined through purely geometrical considerations. Experimental analysis of the orientation of domain walls and period of the triangular network would, on the one hand, contribute to understanding of the interlayer interaction of graphene layers, and, on the other hand, serve for detection of relative strains and rotation between the layers. Vice versa external strains can be used to control the parameters of the triangular domain wall network and, therefore, electronic properties of twisted bilayer graphene.

cond-mat.mes-hall↗