We report inelastic light scattering experiments on CaFe_2As_2 in the temperature range of 4 to 290 K. In in-plane polarizations two Raman-active phonon modes are observed at 189 and 211 cm-1, displaying A_1g and B_1g symmetries, respectively. Upon heating through the tetragonal-to-orthorhombic transition at about T_S=173 K, the B_1g phonon undergoes a discontinuous drop of the frequency by 4 cm-1 whereas the A_1g phonon shows a suppression of the integrated intensity. Their linewidth increases strongly with increasing temperature and saturates above T_S. This suggests (i) a first-order structural phase transition and (ii) a drastic change of charge distribution within the FeAs plane through T_S.
We performed optical studies on CaFeAsF single crystals, a parent compound of the 1111-type iron-based superconductors that undergoes a structural phase transition from tetragonal to orthorhombic at $T_s$ = 121 K and a magnetic one to a spin density wave (SDW) state at $T_N$ = 110 K. In the low temperature optical conductivity spectrum, after the subtraction of a narrow Drude peak, we observe a pronounced singularity around 300 cm$^{-1}$ that separates two regions of quasilinear conductivity. We outline that these characteristic absorption features are signatures of Dirac fermions, similar to …
We report the complex dielectric function of high-quality $A\textrm{Fe}_2\textrm{As}_2$, ($A$=Ca, Sr, Ba) single crystals with $T_{\mathrm{N}}\approx150\ \textrm{K}$, $200\ \textrm{K}$, and $138\ \textrm{K}$, respectively, determined by broadband spectroscopic ellipsometry at temperatures $10\leq T\leq300\ \textrm{K}$ and wavenumbers from $100\ \textrm{cm}^{-1}$ to $52000\ \textrm{cm}^{-1}$. In $\textrm{CaFe}_2\textrm{As}_2$ we identify the optical spin-density--wave gap $2Δ_{\mathrm{SDW}}\approx1250\ \textrm{cm}^{-1}$. The $2Δ_{\mathrm{SDW}}/(k_{\mathrm{B}}T_{\mathrm{N}})$ ratio, characterizi…
We report inelastic light scattering studies on Ca(Fe0.97Co0.03)2As2 in a wide spectral range of 120-5200 cm-1 from 5K to 300K, covering the tetragonal to orthorhombic structural transition as well as magnetic transition at Tsm ~ 160K. The mode frequencies of two first-order Raman modes B1g and Eg, both involving displacement of Fe atoms, show sharp increase below Tsm. Concomitantly, the linewidths of all the first-order Raman modes show anomalous broadening below Tsm, attributed to strong spin-phonon coupling. The high frequency modes observed between 400-1200 cm-1 are attributed to the elect…
We present a detailed temperature dependent Raman light scattering study of optical phonons in Ba{1-x}K{x}Fe{2}As{2} (x ~ 0.28, superconducting Tc ~ 29 K), Sr{1-x}K{x}Fe{2}As{2} (x ~ 0.15, Tc ~ 29 K) and non-superconducting BaFe{2}As{2} single crystals. In all samples we observe a strong continuous narrowing of the Raman-active Fe and As vibrations upon cooling below the spin-density-wave transition Ts. We attribute this effect to the opening of the spin-density-wave gap. The electron-phonon linewidths inferred from these data greatly exceed the predictions of ab-initio density functional calc…
We report pressure tuned Raman and x-ray diffraction data of Bi1.98Sr2.06Y0.68Cu2O8 revealing a critical pressure at 21 GPa with anomalies in six physical quantities: electronic Raman background, electron-phonon coupling, spectral weight transfer from high to low frequency, density dependent behaviour of phonon and magnon frequencies, and a compressibility change in the c-axis. For the first time in a cuprate, mobile charge carriers, lattice, and magnetism all show anomalies at a distinct critical pressure in the same experimental setting. Furthermore, the Raman spectral changes are similar to…
We present a detailed temperature-dependent Raman light scattering study of optical phonons in molecular-beam-epitaxy-grown films of the electron-doped superconductor La_{2-x}Ce_{x}CuO_{4} close to optimal doping (x ~ 0.08, T_c = 29 K and x ~ 0.1, T_c = 27 K). The main focus of this work is a detailed characterization and microstructural analysis of the films. Based on micro-Raman spectroscopy in combination with x-ray diffraction, energy-dispersive x-ray analysis, and scanning electron microscopy, some of the observed phonon modes can be attributed to micron-sized inclusions of Cu_{2}O. In th…
Polarized Raman spectra of non-superconducting SrFe$_2$As$_2$ and superconducting K$_{0.4}$Sr$_{0.6}$Fe$_2$As$_2$ ($T_c = 37$ K) are reported. All four phonon modes (A$_{1g}$ + B$_{1g}$ + 2E$_g$) allowed by symmetry, are found and identified. Shell model gives reasonable description of the spectra. No detectable anomalies are observed near the tetragonal-to-orthorhombic transition in SrFe$_2$As$_2$ or the superconducting transition in K$_{0.4}$Sr$_{0.6}$Fe$_2$As$_2$.
We report an investigation of the lattice dynamical properties of LiFeAs using inelastic light scattering. Five out of the six expected phonon modes are observed. The temperature evolution of their frequencies and linewidths is in good agreement with an anharmonic-decay model. We find no evidence for substantial electron-phonon coupling, and no superconductivity-induced phonon anomalies.
We report interesting anomalies in the temperature dependent Raman spectra of FeSe$_{0.82}$ measured from 3K to 300K in the spectral range from 60 to 1800 cm$^{-1}$ and determine their origin using complementary first-principles density functional calculations. A phonon mode near 100 cm$^{-1}$ exhibits a sharp increase by $\sim$ 5% in frequency below a temperature T$_s$ ($\sim$ 100 K) attributed to strong spin-phonon coupling and onset of short-range antiferromagnetic order. In addition, two high frequency modes are observed at 1350 cm$^{-1}$ and 1600 cm$^{-1}$, attributed to electronic Raman …
Sc5Rh6Sn18 with a cage-type quasiskutterudite crystal lattice and type II superconductivity, with superconducting transition temperature Tc = 4.99 K, was investigated under hydrostatic high-pressure (HP) using electrical transport, synchrotron X-ray diffraction (XRD) and Raman spectroscopy. Our data show that HP enhance the metallic nature and Tc of the system. Tc is found to show a continuous increase reaching to 5.24 K at 2.5 GPa. Athough the system is metallic in nature, Raman spectroscopy investigations at ambient pressure revealed the presence of three weak modes at 165.97, 219.86 and 230…
High purity niobium (Nb), subjected to the processing methods used in the fabrication of superconducting RF cavities, displays micron-sized surface patches containing excess carbon. High-resolution transmission electron microscopy and electron energy-loss spectroscopy measurements are presented which reveal the presence of nanoscale NbC coherent precipitates in such regions. Raman backscatter spectroscopy on similar surface regions exhibit spectra consistent with the literature results on bulk NbC but with significantly enhanced two-phonon scattering. The unprecedented strength and sharpness o…
Vibrational properties of iron-chalcogenide superconductor K$_{0.75}$Fe$_{1.75}$Se$_{2}$ with $T_{c}\sim$ 30 K have been measured by Raman and optical spectroscopies over temperature range of 3-300 K. Sample undergoes \textit{I4/m} $\to $ \textit{I4} structural phase transition accompanied by loss of inversion symmetry at $T_{1}$, below 250 K, observed as appearance of new fully-symmetric Raman mode at $\sim$ 165 cm$^{-1}$. Small vibration mode anomalies are also observed at $T_{2}\sim$ 160 K. From first-principles vibrational analysis of antiferromagnetic K$_{0.8}$Fe$_{1.6}$Se$_{2}$ utilizing…
Analysis of the a-b plane optical conductivity $σ_{ab}$ for both twinned and untwinned YBa$_{2}$Cu$_{3}$O$_{7-δ}$ as a function of temperature and doping shows that below a well defined temperature T*, a dip in the spectrum systematically appears separating the infrared charge excitation spectrum into two components with distinct energy scales. The change from monotonic behaviour in $σ_{ab}$ is found to be concurrent with the onset of phonon anomalies in Raman and infrared spectra below T*. The optical data are suggested to be evidence for the appearance of an inhomogeneous distribution of car…
Inelastic light (Raman) scattering has been used to study electronic excitations and phonon anomalies in detwinned, slightly overdoped YBa$_2$Cu$_3$O$_{6.95}$ and moderately overdoped Y$_{0.85}$Ca$_{0.15}$Ba$_2$Cu$_3$O$_{6.95}$ single crystals. In both samples modifications of the electronic pair-breaking peaks when interchanging the a- and b-axis were observed. The lineshapes of several phonon modes involving plane and apical oxygen vibrations exhibit pronounced anisotropies with respect to the incident and scattered light field configurations. Based on a theoretical model that takes both ele…
Inelastic light scattering studies on single crystal of electron-doped Ca(Fe0.95Co0.05)2As2 superconductor, covering the tetragonal to orthorhombic structural transition as well as magnetic transition at TSM ~ 140 K and superconducting transition temperature Tc ~ 23 K, reveal evidence for superconductivity-induced phonon renormalization; in particular the phonon mode near 260 cm-1 shows hardening below Tc, signaling its coupling with the superconducting gap. All the three Raman active phonon modes show anomalous temperature dependence between room temperature and Tc i.e phonon frequency decrea…
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…
In Raman spectra of cuprate superconductors the gap shows up both directly, via a redistribution of the electronic background, the so-called "2Delta peaks", and indirectly, e.g. via the renormalization of phononic excitations. We use a model that allows us to study the redistribution and the related phonon self-energy effects simultaneously. We apply this model to the B_1g phonon of Y_{1-x}(Pr,Ca)_xBa_2Cu_3O_7 films, where Pr or Ca substitution enables us to investigate under- and overdoped samples. While various self-energy effects can be explained by the strength and energy of the 2Δpeaks, a…
Combined synchrotron angle-dispersive powder diffraction and micro-Raman spectroscopy are used to investigate the pressure-induced lattice instabilities that are accompanied by T$_{\rm c}$ anomalies in YBa$_{\rm 2}$Cu$_{\rm 4}$O$_{\rm 8}$, in comparison with the optimally doped YBa$_{\rm 2}$Cu$_{\rm 3}$O$_{\rm 7-δ}$ and the non-superconducting PrBa$_{\rm 2}$Cu$_{\rm 3}$O$_{\rm 6.92}$. In the first two superconducting systems there is a clear anomaly in the evolution of the lattice parameters and an increase of lattice disorder with pressure, that starts at $\approx3.7 GPa$ as well as irreversi…
Using Raman spectroscopy and transport measurements we investigate thin epitaxial films of Y{1-x}(Pr,Ca)xBa2Cu3O{6+y}. We explore the electronic Raman responses obtained after subtraction of phononic excitations, and the 2Delta peaks that form out of the electronic background below Tc. We find that the energy of the B1g 2Delta peak increases monotonically with decreasing doping until the peaks become unresolvable. In contrast, the peaks in A1g symmetry follow Tc being resolvable in the Pr-doped films. The B2g responses are weak and a 2Delta peak is only detected at the highest doping level. As…
We report Raman light scattering in the phase separated superconducting single crystal Rb0.77Fe1.61Se2 with Tc = 32 K. The spectra have been measured in a wide temperature range 3K -500K. The observed phonon lines from the majority vacancy ordered Rb2Fe4Se5 (245) antiferromagnetic phase with TN= 525 K demonstrate modest anomalies in frequency, intensity and halfwidth at the superconductive phase transition. We identify phonon lines from the minority compressed RbδFe2Se2 (122) conductive phase. The superconducting gap with dx2-y2 symmetry is also detected in our spectra. In the range 0-600 cm-1…
Multiorbital character of the density wave in trilayer nickelate superconductors
Max-Planck-Institute for Solid State Research（马克斯·普朗克固体研究所）；Facultad de Ciencias Exactas, Ingeniería y Agrimensura and Instituto de Física Rosario (UNR-CONICET)（罗萨里奥大学精确科学、工程与测量学院及罗萨里奥物理研究所（UNR-CONICET））；RIKEN Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所跨学科理论与数学科学中心 (iTHEMS)）
Using resonant X-ray diffraction and Raman spectroscopy, we study charge correlations and lattice dynamics in two model cuprates, HgBa$_{2}$CuO$_{4+δ}$ and HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$. We observe a maximum of the characteristic charge order temperature around the same hole concentration ($p \approx 0.09$) in both compounds, and concomitant pronounced anomalies in the lattice dynamics that involve the motion of atoms in and/or adjacent to the CuO$_2$ layers. These anomalies are already present at room temperature, and therefore precede the formation of the static charge correlations, and we a…
Hydrostatic pressure Raman measurements have been carried out on the SmFeAsO series of oxypnictides with varying amount of doping (F substitution for O and Co for Fe) and transition temperature (T_{c}), in order to investigate lattice modifications and their connection to doping and superconductivity. Synchrotron XRD data on some of these compounds indicated that at low doping the lattice constants vary smoothly with pressure, but with increasing F concentration there is a deviation from the normal equation of state and these effects are related with modifications in the superconducting FeAs4 …
The lattice properties at low temperatures of two samples of NdFeAsO1-xFx (x=0.05 and 0.25) have been examined in order to investigate possible structural phase transition that may occur in the optimally doped superconducting sample with respect to the non-superconducting low-F concentration compound. In order to detect small modifications in the ion displacements with temperature micro-Raman and high resolution synchrotron powder diffraction measurements were carried out. No increase of the width of the (220) or (322) tetragonal diffraction peaks and microstrains could be found in the superco…
We present results of a systematic study of the c axis lattice dynamics in single layer Bi2Sr2CuO6 (Bi2201), bilayer Bi2Sr2CaCu2O8 (Bi2212) and trilayer Bi2Sr2Ca2Cu3O10 (Bi2223) cuprate superconductors. Our study is based on both experimental data obtained by spectral ellipsometry on single crystals and theoretical calculations. The calculations are carried out within the framework of a classical shell model, which includes long-range Coulomb interactions and short-range interactions of the Buckingham form in a system of polarizable ions. Using the same set of the shell model parameters for Bi…
Polarized Raman-scattering spectra of superconducting, single-crystalline FeSe evidence pronounced phonon anomalies with temperature reduction. A large 6.5% hardening of the B_1g(Fe) phonon mode is attributed to the suppression of local fluctuations of the iron spin state with the gradual decrease of the iron paramagnetic moment. The ab-initio lattice dynamic calculations support this conclusion. The enhancement of the low-frequency spectral weight above the structural phase transition temperature T_s and its change below T_s is discussed in relation with the opening of an energy gap between l…
Fermi surface fluctuations and lattice instabilities in the 2D metallic kagome superconductor CsV$_3$Sb$_5$ are elucidated via polarization-resolved Raman spectroscopy. The presence of a weak electronic continuum in high-quality samples marks the cross-over into the charge-density-wave (CDW) ordered phase, while impurity-rich samples promote strong defect-induced electronic scattering processes that affect the coherence of the CDW phase. CDW-induced phonon anomalies appear below $T_{\mathrm{CDW}}$, with emergent $C2$ symmetry for one of the CDW amplitude modes, alluding to nematicity. In conju…
The combination of non-trivial band topology and symmetry breaking phases gives rise to novel quantum states and phenomena such as topological superconductivity, quantum anomalous Hall effect and axion electrodynamics. Evidence of intertwined charge density wave (CDW) and superconducting order parameters has recently been observed in a novel kagome material AV3Sb5 (A=K,Rb,Cs) that features a Z2 topological invariant in the electronic structure. However, the origin of the CDW and its intricate interplay with topological state has yet to be determined. Here, using hard x-ray scattering, we demon…
