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Z. V. Popović

Publications and source records attributed to Z. V. Popović.

17 recordsLinked to original sources

Competition of disorder and electron-phonon coupling in 2H-TaSe$_{2-x}$S$_x$ ($0\le x\le 2$) as evidenced by Raman spectroscopy

The vibrational properties of 2H-TaSe$_{2-x}$S$_x$ ($0 \le x \le 2$) single crystals were probed using Raman spectroscopy and density functional theory calculations. The end members revealed two out of four symmetry-predicted Raman active modes, together with the pronounced two-phonon structure, attributable to the enhanced electron-phonon coupling. Additional peaks become observable due to crystallographic disorder for the doped samples. The evolution of the E$_{2g}^2$ mode Fano parameter reveals that the disorder has weak impact on electron-phonon coupling, which is also supported by the persistence of two-phonon structure in doped samples. As such, this research provides thorough insights into the lattice properties, the effects of crystallographic disorder on Raman spectra, and the interplay of this disorder with the electron-phonon coupling in 2H-TaSe$_{2-x}$S$_x$ compounds.

cond-mat.mtrl-sci↗

Probing charge density wave phases and the Mott transition in $1T$-TaS$_2$ by inelastic light scattering

We present a polarization-resolved, high-resolution Raman scattering study of the three consecutive charge density wave (CDW) regimes in $1T$-TaS$_2$ single crystals, supported by \textit{ab initio} calculations. Our analysis of the spectra within the low-temperature commensurate (C-CDW) regime shows $\mathrm{P3}$ symmetry of the system, thus excluding the previously proposed triclinic stacking of the "star-of-David" structure, and promoting trigonal or hexagonal stacking instead. The spectra of the high-temperature incommensurate (IC-CDW) phase directly project the phonon density of states due to the breaking of the translational invariance, supplemented by sizeable electron-phonon coupling. Between 200 and 352\,K, our Raman spectra show contributions from both the IC-CDW and the C-CDW phase, indicating their coexistence in the so-called nearly-commensurate (NC-CDW) phase. The temperature-dependence of the symmetry-resolved Raman conductivity indicates the stepwise reduction of the density of states in the CDW phases, followed by a Mott transition within the C-CDW phase. We determine the size of the Mott gap to be $Ω_{\rm gap}\approx 170-190$ meV, and track its temperature dependence.

cond-mat.str-el↗

Lattice dynamics and phase transitions in Fe$_{3-x}$GeTe$_2$

We present Raman spectroscopy measurements of the van der Waals bonded ferromagnet Fe$_{3-x}$GeTe$_2$, together with lattice dynamics. Four out of eight Raman active modes are observed and assigned, in agreement with numerical calculations. The energies and line-widths of the observed modes display an unconventional temperature dependence at about 150 K and 220 K, followed by the nonmonotonic evolution of the Raman continuum. Whereas the former can be related to the magnetic phase transition, the origin of the latter anomaly remains an open question.

cond-mat.mtrl-sci↗

Evidence of spin-phonon coupling in CrSiTe$_3$

We present the Raman scattering results on layered 2D semiconducting ferromagnetic compound CrSiTe$_3$. Four Raman active modes, predicted by symmetry, have been observed and assigned. The experimental results are supported by DFT calculations. The self-energies of the $A_g^3$ and the $E_g^3$ symmetry modes exhibit unconventional temperature evolution around 180 K. In addition, the doubly degenerate $E_g^3$ mode shows clear change of asymmetry in the same temperature region. The observed behavior is consistent with the presence of the previously reported short-range magnetic order and the strong spin-phonon coupling.

cond-mat.mtrl-sci↗

Lattice dynamics and phase transition in CrI$_3$ single crystals

The vibrational properties of $\mathrm{CrI_3}$ single crystals were investigated using Raman spectroscopy and were analyzed with respect to the changes of the crystal structure. All but one mode are observed for both the low-temperature $R\bar{3}$ and the high-temperature C2/$m$ phase. For all observed modes the energies and symmetries are in good agreement with DFT calculations. The symmetry of a single-layer was identified as $p\bar{3}1/m$. In contrast to previous studies we observe the transition from the $R\bar{3}$ to the $\mathrm{C2}/m$ phase at 180\,K and find no evidence for coexistence of both phases over a wide temperature range.

cond-mat.mtrl-sci↗

Phonon anomalies in FeS

We present results from light scattering experiments on tetragonal FeS with the focus placed on lattice dynamics. We identify the Raman active A1g and B1g phonon modes, a second order scattering process involving two acoustic phonons, and contributions from potentially defect-induced scattering. The temperature dependence between 300 and 20K of all observed phonon energies is governed by the lattice contraction. Below 20K the phonon energies increase by 0.5-1 cm$^{-1}$ thus indicating putative short range magnetic order. Along with the experiments we performed lattice-dynamical simulations and a symmetry analysis for the phonons and potential overtones and find good agreement with the experiments. In particular, we argue that the two-phonon excitation observed in a gap between the optical branches becomes observable due to significant electron-phonon interaction.

cond-mat.supr-con↗

Small influence of magnetic ordering on lattice dynamics in TaFe$_{1.25}$Te$_3$

Raman scattering spectra of zigzag spin chain TaFe$_{1.25}$Te$_3$ single crystal are presented in a temperature range from 80 to 300 K. Nine Raman active modes of $A_g$ and $B_g$ symmetry are clearly observed and assigned by probing different scattering channels, which is confirmed by lattice dynamics calculations. Temperature dependence of the Raman modes linewidth is mainly governed by the lattice anharmonicity. The only deviation from the conventional behavior is observed for $A_g$ symmetry modes in a vicinity of the magnetic phase transition at $T_N \approx 200$ K. This implies that the electron-phonon interaction weakly changes with temperature and magnetic ordering, whereas small changes in the spectra near the critical temperature can be ascribed to spin fluctuations.

cond-mat.mtrl-sci↗

Raman spectroscopy of K_xCo_{2-y}Se_2 single crystals near the ferromagnet-paramagnet transition

Polarized Raman scattering spectra of the K_xCo_{2-y}Se_2 single crystals reveal the presence of two phonon modes, assigned as of the A_{1g} and B_{1g} symmetry. Absence of additional modes excludes the possibility of vacancy ordering, unlike in K_xFe_{2-y}Se_2. The ferromagnetic (FM) phase transition at T_c\approx 74 K leaves a clear fingerprint on the temperature dependence of the Raman mode energy and linewidth. For T>T_c the temperature dependence looks conventional, driven by the thermal expansion and anharmonicity. The Raman modes are rather broad due to the electron-phonon coupling increased by the disorder and spin fluctuation effects. In the FM phase the phonon frequency of both modes increases, while an opposite trend is seen in their linewidth: the A_{1g} mode narrows in the FM phase, whereas the B_{1g} mode broadens. We argue that the large asymmetry and anomalous frequency shift of the B_{1g} mode is due to the coupling of spin fluctuations and vibration. Our density functional theory (DFT) calculations for the phonon frequencies agree rather well with the Raman measurements, with some discrepancy being expected since the DFT calculations neglect the spin fluctuations.

cond-mat.mtrl-sci↗

Evidence of superconductivity-induced phonon spectra renormalization in alkali-doped iron selenides

Polarized Raman scattering spectra of superconducting K$_x$Fe$_{2-y}$Se$_2$ and nonsuperconducting K$_{0.8}$Fe$_{1.8}$Co$_{0.2}$Se$_2$ single crystals were measured in a temperature range from 10 K up to 300 K. Two Raman active modes from the $I4/mmm$ phase and seven from the $I4/m$ phase are observed in frequency range from 150 to 325 cm$^{-1}$ in both compounds, suggesting that K$_{0.8}$Fe$_{1.8}$Co$_{0.2}$Se$_2$ single crystal also has two-phase nature. Temperature dependence of Raman mode energy is analyzed in terms of lattice thermal expansion and phonon-phonon interaction. Temperature dependence of Raman mode linewidth is dominated by temperature-induced anharmonic effects. It is shown that change of Raman mode energy with temperature is dominantly driven by thermal expansion of the crystal lattice. Abrupt change of the A$_{1g}$ mode energy near $T_C$ was observed in K$_x$Fe$_{2-y}$Se$_2$, whereas it is absent in non-superconducting K$_{0.8}$Fe$_{1.8}$Co$_{0.2}$Se$_2$. Phonon energy hardening at low temperatures in the superconducting sample is a consequence of superconductivity-induced redistribution of the electronic states below critical temperature.

cond-mat.mtrl-sci↗

Lattice dynamics of KNi2Se2

We report the first principle calculations of the lattice dynamics of KNi$_{2}$Se$_2$ together with the Raman scattering study.\ We have observed three out of four Raman active modes predicted by the factor group analysis. Calculated phonon frequencies are in good agreement with experimental findings.\ Contrary to its iron counterpart (K$_x$Fe$_{2-y}$Se$_2$), K$_{0.95}$Ni$_{1.86}$Se$_2$ does not show vacancy ordering.

cond-mat.supr-con↗

Probing IrTe2 crystal symmetry by polarized Raman scattering

Polarized Raman scattering measurements on IrTe$_2$ single crystals carried out over 15~K - 640~K temperature range, and across the structural phase transition, reveal new insights regarding the crystal symmetry.\ In the high temperature regime three Raman active modes are observed at all studied temperatures above the structural phase transition, rather than two as predicted by the factor group analysis for the assumed $P\bar{3}m1$ symmetry. This indicates that the actual symmetry of the high temperature phase is lower than previously thought.\ Observation of an additional E$_g$ mode at high temperature can be explained by doubling of the original trigonal unit cell along the $c$-axis and within the $P\bar{3}c1$ symmetry.\ In the low temperature regime (below 245 K) the new Raman modes appear as a consequence of the symmetry lowering phase transition and corresponding increase of the primitive cell.\ All the modes observed below the phase transition temperature can be assigned within the monoclinic crystal symmetry.\ Temperature dependence of the Raman active phonons in both phases are mainly driven by anharmonicity effects. The results call for reconsideration of the crystallographic phases of IrTe$_2$.

cond-mat.supr-con↗

Phonon and magnetic dimer excitations in Fe-based S=2 spin ladder compound BaFe$_2$Se$_2$O

Raman scattering spectra of new Fe-based S=2 spin ladder compound BaFe$_2$Se$_2$O are measured in a temperature range between 15 K and 623 K. All six A$_{1g}$ and two B$_{1g}$ Raman active modes of BaFe$_2$Se$_2$O, predicted by the factor-group analysis, have been experimentally observed at energies that are in a rather good agreement with the lattice dynamics calculation. The antiferromagnetic long-range spin ordering in BaFe$_2$Se$_2$O below $T_N$=240 K leaves a fingerprint both in the A$_{1g}$ and B$_{1g}$ phonon mode linewidth and energy. In the energy range between 400 and 650 cm$^{-1}$ we have observed magnetic excitation related structure in the form of magnon continuum, with the peaks corresponding to the singularities in the one dimensional density of magnon states. The onset value of magnetic continuum (2$Δ_{S}$) is found at about 437 cm$^{-1}$ at 15 K. The magnetic continuum disappears at about 623 K, which lead us to conclude that the short-range magnetic ordering in BaFe$_2$Se$_2$O exists apparently up to 2.6$T_N$.

cond-mat.mtrl-sci↗

Evidence for electron-phonon interaction in Fe$_{1-x}$M$_{x}$Sb$_{2}$ (M=Co, Cr) single crystals

We have measured polarized Raman scattering spectra of the Fe$_{1-x}$Co$_{x}$Sb$_{2}$ and Fe$_{1-x}$Cr$_{x}$Sb$_{2}$ (0$\leq x\leq $0.5) single crystals in the temperature range between 15 K and 300 K. The highest energy $B_{1g}$ symmetry mode shows significant line asymmetry due to phonon mode coupling width electronic background. The coupling constant achieves the highest value at about 40 K and after that it remains temperature independent. Origin of additional mode broadening is pure anharmonic. Below 40 K the coupling is drastically reduced, in agreement with transport properties measurements. Alloying of FeSb$_2$ with Co and Cr produces the B$_{1g}$ mode narrowing, i.e. weakening of the electron-phonon interaction. In the case of A$_{g}$ symmetry modes we have found a significant mode mixing.

cond-mat.str-el↗

Evidence of phonon-charge-density-waves coupling in ErTe$_3$

The vibrational properties of ErTe$_3$ were investigated using Raman spectroscopy and analyzed on the basis of peculiarities of the RTe$_3$ crystal structure. Four Raman active modes for the undistorted structure, predicted by factor-group analysis, are experimentally observed and assigned according to diperiodic symmetry of the ErTe$_3$ layer. By analyzing temperature dependence of the Raman mode energy and intensity we have provided the clear evidence that all Raman modes, active in the normal phase, are coupled to the charge density waves. In addition, new modes have been observed in the distorted state.

cond-mat.str-el↗

Orbital Dimerization and Dynamic Jahn-Teller Effect in NaTiSi$_2$O$_6$

We study with the Raman scattering technique two types of phase transitions in the pyroxene compounds NaMSi$_2$O$_6$ (with M=Ti, V, and Cr). In the quasi one-dimensional S=1/2 system NaTiSi$_2$O$_6$ we observe anomalous high-temperature phonon broadening and large changes of the phonon energies and line-widths across the phase transition at 210 K. The phonon anomalies originate from an orbital order-disorder phase transition and these results --combined with theoretical considerations-- indicate that the high temperature dynamical Jahn-Teller phase of NaTiSi$_2$O$_6$ exhibits a spontaneous breaking of translational symmetry into a dimerized, Jahn-Teller distorted, orbital ordered state under the formation of spin valence bonds. In S=1 NaVSi$_2$O$_6$ orbital degrees of freedom are strongly suppressed and the magnetic excitations are well described within a Heisenberg model, indicating that at T$_N$=19K this system orders antiferromagnetically.

cond-mat.str-el↗

Polarized far-infrared and Raman spectra of SrCuO2 single crystals

We measured polarized far-infrared reflectivity and Raman scattering spectra of SrCuO$_2$ single crystals. The frequencies for infrared-active modes were determined using an oscillator-fitting procedure of reflectivity data. The Raman spectra were measured at different temperatures using several laser energies $ω_L$. In addition to eight of twelve Raman active modes, predicted by factor-group analysis, we observed a complex structure in the Raman spectra for polarization parallel to the {\bf c}-axis, which consists of Raman-allowed A$_g$ symmetry modes, and B$_{1u}$ LO infrared-active (Raman-forbidden) modes of the first and higher order as well as their combinations. The Raman-forbidden modes have a stronger intensity at higher $ω_L$ than the Raman-allowed ones. In order to explain this resonance effect, we measured the dielectric function and optical reflection spectra of SrCuO$_2$ in the visible range. We show that the Raman-allowed A$_g$ symmetry modes are resonantly enhanced when a laser energy is close to $E_0$, while Raman-forbidden (IR-active) modes resonate strongly for laser line energies close to the electronic transition of higher energy gaps.

cond-mat.str-el↗

Optical Properties of the Spin-Ladder Compound Sr_{14}Cu_{24}O_{41}

We report the measurements of the pseudodielectric function, far-infrared reflectivity and Raman scattering spectra in Sr_{14}Cu_{24}O_{41} single crystal. We study the lattice and the spin dynamics of the Cu$_2$O$_3$ spin ladders and CuO$_2$ chains of this compound. The ellipsometric and the optical reflectivity measurements yield the gap values of 1.4 eV, 1.86 eV, 2.34 eV (2.5 eV) for the ladders (chains) along the {\bf c}-axis and 2.4 eV along the {\bf a}-axis. The electronic structure of the Cu$_2$O$_3$ ladders is analyzed using tight-binding approach for the correlated electron systems. The correlation gap value of 1.4 eV is calculated with the transfer energy (hopping) parameters $t=t_{0}$=0.26 eV, along and perpendicular to legs, $t_{xy}$=0.026 eV (interladder hopping) and U=2.1 eV, as a Coulomb repulsion. The optical parameters of the infrared active phonons and plasmons are obtained by oscillator fitting procedure of the reflectivity spectra. Raman scattering spectra are measured at different temperatures using different laser line energies. The two-magnon peak is observed at about 2880 cm$^{-1}$. At temperatures below 150 K the new infrared and Raman modes appear due to the charge ordering.

cond-mat.str-el↗