arXiv subjects

Volodymyr Turkowski

Publications and source records attributed to Volodymyr Turkowski.

At least 19 recordsLinked to original sources

arXiv2024

Impurity effects in twisted carbon nanotubes

We consider electronic spectra of twisted carbon nanotubes and their perturbation by impurity atoms absorbed at different positions on nanotube surface within the framework of Anderson hybrid model. A special attention is given to the cases when 1D Weyl (massless Dirac) modes are present in the nanotube spectrum and their hybridization with localized impurity states produces, with growing impurity concentration c, onset of a mobility gap near the impurity level and then opening, at yet higher c, of some narrow range of delocalized states within this mobility gap. Such behaviors are compared with similar effects in the previously studied 2D graphene, carbon nanoribbons, and non-twisted carbon nanotubes. Some possible practical applications are discussed.

cond-mat.mes-hall↗

arXiv2023

Thickness dependence of superconductivity in FeSe films

The films of FeSe on substrates have attracted attention because of their unusually high-temperature (Tc) superconducting properties whose origins continue to be debated. To disentangle the competing effects of the substrate and interlayer and intralayer processes, we present here results of density functional theory (DFT)-based analysis of the electronic structure of unsupported FeSe films consisting of 1 to 5 layers (1L-5L). Furthermore, by solving the Bardeen-Schrieffer-Cooper (BCS) equation with spin-wave exchange attraction derived from the Hubbard model, we find the superconducting critical temperature Tc for 1L-5L and bulk FeSe systems in reasonable agreement with experimental data. Our results point to the importance of correlation effects in superconducting properties of single- and multi-layer FeSe films, independently of the role of substrate.

cond-mat.supr-con↗

arXiv2023

Dark exciton energy splitting in monolayer WSe2: insights from time-dependent density-functional theory

We present here a formalism based on time-dependent density-functional theory (TDDFT) to describe characteristics of both intra- and inter-valley excitons in semiconductors, the latter of which had remained a challenge. Through the usage of an appropriate exchange-correlation kernel (nanoquanta), we trace the energy difference between the intra- and inter-valley dark excitons in monolayer (1L) WSe2 to the domination of the exchange part in the exchange-correlation energies of these states. Furthermore, our calculated transition contribution maps establish the momentum resolved weights of the electron-hole excitations in both bright and dark excitons thereby providing a comprehensive understanding of excitonic properties of 1L WSe2. We find that the states consist of hybridized excitations around the corresponding valleys which leads to brightening of the dark excitons, i.e., significantly decreasing their lifetime which is reflected in the PL spectrum. Using many-body perturbation theory, we calculate the phonon contribution to the energy bandgap and the linewidths of the excited electrons, holes and (bright) exciton to find that as the temperature increases the bandgap significantly decreases, while the linewidths increase. Our work paves for describing the ultrafast charge dynamics of transition metal dichalcogenide within an ab initio framework.

cond-mat.mtrl-sci↗

arXiv2023

Mapping Spin Interactions from Conductance Peak Splitting in Coulomb Blockade

We investigate the transport properties of a quantum dot coupled to leads interacting with a multi-spin system using the generalized master equation within the Coulomb blockade regime. We find that if two states for each scattering region electron manifold are included, several signatures of the interacting spin system appear in steady-state transport properties. We provide a theoretical mapping of differential conductance peak signatures and all spin Hamiltonian parameters related to the inclusion of excited state transitions between uncharged and charged electron manifolds. Our predictions describe a scheme of only using a quantum dot and differential conductance to measure magnetic anisotropy, inter-spin exchange coupling, exchange coupling between the spin system and itinerant electron, and applied magnetic field response.

cond-mat.mes-hall↗

arXiv2021

Electron Thermalization and Relaxation in Laser-Heated Nickel by Few-Femtosecond Core-Level Transient Absorption Spectroscopy

Direct measurements of photoexcited carrier dynamics in nickel are made using few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy at the nickel M$_{2,3}$ edge. It is observed that the core-level absorption lineshape of photoexcited nickel can be described by a Gaussian broadening ($σ$) and a red shift ($ω_{s}$) of the ground state absorption spectrum. Theory predicts, and the experimental results verify that after initial rapid carrier thermalization, the electron temperature increase ($ΔT$) is linearly proportional to the Gaussian broadening factor $σ$, providing quantitative real-time tracking of the relaxation of the electron temperature. Measurements reveal an electron cooling time for 50 nm thick polycrystalline nickel films of 640$\pm$80 fs. With hot thermalized carriers, the spectral red shift exhibits a power-law relationship with the change in electron temperature of $ω_{s}\proptoΔT^{1.5}$. Rapid electron thermalization via carrier-carrier scattering accompanies and follows the nominal 4 fs photoexcitation pulse until the carriers reach a quasi-thermal equilibrium. Entwined with a <6 fs instrument response function, carrier thermalization times ranging from 34 fs to 13 fs are estimated from experimental data acquired at different pump fluences and it is observed that the electron thermalization time decreases with increasing pump fluence. The study provides an initial example of measuring electron temperature and thermalization in metals in real time with XUV light, and it lays a foundation for further investigation of photoinduced phase transitions and carrier transport in metals with core-level absorption spectroscopy.

cond-mat.mtrl-sci↗

arXiv2020

Spatially non-homogeneous metallization of VO2: a TDDFT+DMFT analysis

We provide insights into the atomistic details of the ultrafast spatially-resolved breakdown of the insulating M1 phase in bulk VO2 employing an ab initio technique based on time-dependent density-functional theory and dynamical mean-field theory (DMFT-TDDFT). We find that the system is initially metallized preferentially along the vanadium-dimer chains (CR axis), with a subsequent growth of CR-elongated metallic bubbles. Moreover, we trace the breakdown of the insulating phase to two types of oxygen atoms, resulting from vanadium dimerization, which produce an unusual charge-density modulation in the oxygen-atom chains with significant charge transfer to the inter-dimer distance. These results are in qualitative agreement with experimental data and shed light on the interplay between valence charge and lattice structure and its role in the ultrafast response of strongly correlated insulators.

cond-mat.str-el↗

arXiv2020

Ultrafast charge dynamics and photoluminescence in bilayer MoS2

Our examination of the interplay of ultrafast charge dynamics and electron-phonon interaction in bilayer MoS2 provides a microscopic basis for understanding the features (two peaks) in the emission spectrum. We demonstrate that while the initial accumulation of excited charge occurs at and near the Q point of the two-dimensional Brillioun zone, emission takes place predominantly through two pathways: direct charge recombination at the K point and indirect phonon-assisted recombination of electrons at the K valley and holes at Γ hill of the Brillouin zone. Analysis of the wave vector dependencies of the electron-phonon interaction traces the higher energy peak to phonon-assisted relaxation of the excited electrons from the Q to the K valley in the conduction band. Our results thus reveal the importance of ultrafast charge dynamics in understanding photoemissive properties of a few-layer transition-metal dichalcogenide. These calculations are based on time dependent density functional theory in the density matrix formulation.

cond-mat.mtrl-sci↗

arXiv2020

Excited states in hydrogenated single-layer MoS$_2$

We calculate the excitation spectrum of single-layer MoS$_2$ at several hydrogen coverages by using a method based on first-principles Density-Matrix Time-Dependent Density-Functional Theory (TDDFT). Our results show that the fully hydrogenated system is metallic, while in the low-coverage limit the spectrum of single-layer MoS$_2$ includes spin-polarized partially filled localized mid-gap states. These states arise from s-orbitals of H atoms which make a tilted bond with the surface S atoms. The calculated absorption spectrum of the system reveals standard excitonic peaks, which correspond to the bound valence-band hole and conduction-band electron, as well as excitonic peaks that involve the mid-gap charges. As in the case of pristine single-layer MoS$_2$, binding energies of the excitons of the hydrogenated system are found to be relatively large (few tens of meV), making their experimental detection facile and suggesting hydrogenation as a knob for tuning the optical properties of single-layer MoS$_2$. Importantly, we find hydrogenation to suppress visible light photoluminescence, in agreement with experimental observations. As an aside, we contrast the effects of hydrogen coverage to that of the next two elements in the same column of the periodic table (the lightest metals), Li and Na, on the spectral properties of single-layer MoS$_2$ which lead instead to the formation of n-doped non-magnetic semiconductors that do not allow excitonic states.

cond-mat.mtrl-sci↗

arXiv2019

Ultrafast demagnetization dynamics in Ni: role of electron correlations

Experimental observations of the ultrafast (less than 50 fs) demagnetization of Ni have so far defied theoretical explanations particularly since its spin-flipping time is much less than that resulting from spin-orbit and electron-lattice interactions. Through the application of an approach that benefits from spin-flip time-dependent density-functional theory and dynamical mean-field theory, we show that proper inclusion of electron correlations and memory (time-dependence of electron-electron interaction) effects leads to demagnetization at the femtosecond scale, in good agreement with experimental observations. Furthermore, our calculations reveal that this ultrafast demagnetization results mainly from spin-flip transitions from occupied to unoccupied orbitals implying a dynamical reduction of exchange splitting. These conclusions are found to be valid for a wide range of laser pulse amplitudes. They also pave the way for ab initio investigations of ultrafast charge and spin dynamics in a variety of quantum materials in which electron correlations may play a definitive role.

cond-mat.str-el↗

arXiv2018

Plasmon excitations in mixed metallic nanoarrays

We study the plasmonic properties of arrays of atomic chains which comprise noble (Cu, Ag, and Au) and transition (Pd, Pt) metal atoms using time-dependent density-functional theory. We show that the response to the electromagnetic radiation is related to both physics, the geometry-dependent confinement of sp-valence electrons, and chemistry, the energy position of d-electrons in the different atomic species and the hybridization between d and sp electrons. As a result it is possible to tune the position of the surface plasmon resonance, split it to several peaks, and eventually achieve broadband absorption of radiation. Mixing the arrays with transition metals can strongly attenuate the plasmonic behaviour. We analyze the origin of these phenomena and show that they arise from rich interactions between single-particle electron-hole and collective electron excitations. The tunability of the plasmonic response of arrays of atomic chains, which can be realized on solid surfaces, opens wide possibilities for their applications. In the present study we obtain guidelines how the desired properties can be achieved.

cond-mat.mes-hall↗

arXiv2015

Magnetic anisotropy of FePt nanoparticles

We carry out a systematic theoretical investigation of Magneto Crystalline Anisotropy (MCA) of L10 FePt clusters with alternating Fe and Pt planes along the (001) direction. We calculate the structural relaxation and magnetic moment of each cluster by using ab initio spin-polarized density functional theory (DFT), and the MCA with both spin-polarized DFT (including spin-orbit coupling self-consistently) and the torque method. We find that the MCA of any composite structure of a given size is enhanced with respect to that of the same-sized pure Pt or pure Fe cluster as well as to that of any pair of Fe and Pt atoms in bulk L10 FePt. This enhancement results from the hybridization we observe between the 3d orbital of the Fe atoms and the 5d orbital of their Pt neighbors. This hybridization, however, affects the electronic properties of the component atoms in significantly different ways. While it somewhat increases the spin moment of the Fe atoms, it has little effect on their orbital moment; at the same time, it greatly increases both the spin and orbital moment of the Pt atoms. Given the fact that the spin-orbit coupling (SOC) constant of Pt is about 7 times greater than that of Fe, this Fe-induced jump in the orbital moment of the Pt atoms produces the increase in MCA of the composite structures over that of their pure counterparts. That any composite structure exhibits higher MCA than bulk L10 FePt results from the lower coordination of Pt atoms in the cluster, whether Fe or Pt predominates within it. We also find that bipyramidal clusters whose central layer is Pt have higher MCA than their same-sized counterparts whose central layer is Fe. This results from the fact that Pt atoms in such configurations are coordinated with more Fe atoms than in the latter. By thus participating in more instances of hybridization, they contribute higher orbital moments to the overall MCA of the unit.

cond-mat.mes-hall↗

arXiv2015

Electron-phonon interaction, excitations and ultrafast photoemission from doped monolayer MoS2

We analyze the effect of electron-phonon coupling on photoemission properties and ultrafast response of doped monolayer MoS2. The analysis is based on combined DFT and many-body (Eliashberg theory) approaches. In particular, we have calculated the electronic and phonon spectra, the electron-phonon coupling and the electronic spectral function of the system at different values of doping. We have also analyzed the emissive properties and the response of the system to femtosecond (fs) laser pulses. It is shown that position of the emission peak of undoped system is in agreement with the experimental data if one takes into account the excitonic effects. The results for the self-energy and spectral functions of the doped systems suggest that one can expect ultrafast processes to be important in the system response , which makes the system attractive from the point of view of modern technological applications. Similar to graphene, the doped system demonstrates ultrafast (fs) relaxation of the electronic subsystem when excited by fs pulses, and a high ultrafast phonon relaxation-induced spectral fluence of visible light emission. Together with high carrier mobility, these features of monolayer MoS2 might be used in modern optoelectronic technologies.

cond-mat.mtrl-sci↗

arXiv2014

Nonadiabatic exchange-correlation kernel for strongly correlated materials

We formulate a rigorous method for calculating a nonadiabatic (frequency-dependent) exchange-correlation (XC) kernel required for correct description of both equilibrium and nonequilibrium properties of strongly correlated systems within Time-Dependent Density Functional Theory (TDDFT). To do so we use the expression for charge susceptibility provided by Dynamical Mean Field Theory (DMFT) for the effective multi-orbital Hubbard Model. We tested our formalism by applying it to the one-band Hubbard model: our nonadiabatic kernel leads to a significant modification of the excitation spectrum, shifting the peak that appears in adiabatic (simplified) solutions and disclosing a new one, in agreement with the DMFT solution. We also used our method to track the nonequilibrium charge-density response of a multi-orbital perovskite Mott insulator, YTiO3, to a perturbation by a femtosecond (fs) laser pulse. The results were quite different from those provided by the corresponding adiabatic formalism. These initial investigations indicate that electron-electron correlations and nonadiabatic features can significantly affect the spectrum and nonequilibrium properties of strongly correlated systems.

cond-mat.str-el↗

arXiv2014

Tuning plasmon excitations in pure and transition metal-doped arrays of noble metal nanochains

We study the plasmonic properties of coupled noble-metal nanochains in the case of different number of coupled chains and doping by different transition-metal (TM) atoms within the time-dependent density-functional theory (TDDFT) approach. We find that as the number of chains in the array increases the plasmon peak shifts from the sub-eV towards the visible range. As doping with TM atoms increases, the visible absorption band broadens, owing to formation of additional plasmon peaks. The optical response is very sensitive to the type of doped atoms, their number and position; in particular, the additional peaks are most pronounced in the case of weak doping when they correspond to local plasmon oscillations around the impurity atom. These effects have a potential to be used in various modern technologies, from sensors to solar cells. Most of the studies of nano-plasmon effects have been focused on alkali- and noble-metal systems with extended s-electron states, while it was believed that doping with TM atoms with their more localized charge as a rule leads to an attenuation of the plasmon modes. We demonstrate that TM atoms can play a constructive role in plasmon generation in small chain systems, and that plasmonic modes can emerge even in some pure TM nanochains.

cond-mat.mes-hall↗

arXiv2014

Time-dependent density-matrix functional theory for trion excitations: application to monolayer MoS2

We study possible optically excited bound states in monolayer MoS2: excitons and trions. For this purpose we formulate and apply a generalized time-dependent density-matrix functional approach for bound states of multiple excitations. The approach was used in the cases of three different types of the exchange-correlation (XC) kernel: 1) two local kernels: a phenomenological contact and the adiabatic local-density approximation (ALDA) (X and XC); 2) gradient-corrected X kernels: GEA, PW91 and PBE; and 3) two long-range (LR) kernels: a phenomenological (Coulomb) and Slater kernels. In the case of exciton, we find that LDA and its gradient-corrected kernels lead to too weak binding energy comparing to the experimental data, while the LR kernels are capable to reproduce the experimental results. Similarly, in the LR case (as well as in the case of local kernel), one can obtain the experimental value of the trion binding energy by taking into account the screening effects. Our results suggest that similar to the excitons, the LR structure of the XC kernel is necessary to describe the trion bound states. Our calculations for the first time confirm theoretically with time-dependent density-functional theory approach that in agreement with experimental data the exciton and trion binding energies are of order of hundreds (excitons) and tenth (trions) meVs, which can be used in different technological applications at the room temperature regime. The approach can be straightforwardly extended on the case of bound states and nonequilibrium response of systems with larger number of bound electrons and holes, including biexcitons.

cond-mat.mes-hall↗

arXiv2013

Time-dependent density-functional theory of exciton-exciton correlations in the nonlinear optical response

We analyze possible nonlinear exciton-exciton correlation effects in the optical response of semiconductors by using a time-dependent density-functional theory (TDDFT) approach. For this purpose, we derive the nonlinear (third-order) TDDFT equation for the excitonic polarization. In this equation, the nonlinear time-dependent effects are described by the time-dependent (non-adiabatic) part of the effective exciton-exciton interaction, which depends on the exchange-correlation (XC) kernel. We apply the approach to study the nonlinear optical response of a GaAs quantum well. In particular, we calculate the 2D Fourier spectra of the system and compare it with experimental data. We find that it is necessary to use a non-adiabatic XC kernel to describe excitonic bound states - biexcitons, which are formed due to the retarded TDDFT exciton-exciton interaction.

cond-mat.mtrl-sci↗

arXiv2013

A DFT+Nonhomogeneous DMFT approach for Finite Systems

For reliable and efficient inclusion of electron-electron correlation effects in nanosystems we propose a combined density-functional-theory/nonhomogeneous dynamical-mean-field-theory (DFT + DMFT) approach which employs an approximate Iterative Perturbative Theory (IPT) impurity solver. The validity of the method is demonstrated by successful examination of the size-dependent magnetic properties of iron nanoparticles containing 11-100 atoms. We show that the DFT+ DMFT solution is in very good agreement with experimental data, in particular it does not lead to the overestimation of magnetization that is found with the DFT and DFT+U techniques. More importantly, we demonstrate that DFT+DMFT approach can be used for accurate and realistic description of nanosystems containing about hundred atoms.

cond-mat.str-el↗

arXiv2013

Nonadiabatic Time-Dependent Spin-Density Functional Theory for strongly correlated systems

We propose a nonadiabatic time-dependent spin-density functional theory (TDSDFT) approach for studying the single-electron excited states and the ultrafast response of systems with strong electron correlations. The correlations are described by the correlation part of the nonadiabatic exchange-correlation (XC) kernel, which is constructed by using some exact results for the Hubbard model of strongly correlated electrons. We demonstrate that the corresponding nonadiabatic XC kernel reproduces main features of the spectrum of the Hubbard dimer and infinite-dimensional Hubbard model, some of which are impossible to obtain within the adiabatic approach. The theory may be applied for DFT study of strongly correlated electron systems in- and out-of-equilibrium, including the important case of nanostructures, for which it leads to a dramatic reduction of necessary computational power.

cond-mat.str-el↗