We report plane-polarized Raman scattering spectra of iron oxypnictide superconductor NdFeAsO$_{1-x}$F$_x$ single crystals with varying fluorine $x$ content. The spectra exhibit sharp and symmetrical phonon lines with a weak dependence on fluorine doping $x$. The temperature dependence does not show any phonon anomaly at the superconducting transition. The Fe related phonon intensity shows a strong resonant enhancement below 2 eV. We associate the resonant enhancement to the presence of an interband transition around 2 eV observed in optical conductivity. Our results point to a rather weak coupling between Raman-active phonons and electronic excitations in iron oxypnictides superconductors.
Raman spectra of polycrystalline NdFeAsO1-xFx (x=0.0, 0.1, 0.2) compound have been systematically investigated as functions of temperature and fluorine concentration. Scanning electron microscopic and Raman microscopic characterization demonstrates that the polycrystalline samples mainly contain two phases, i.e. superconductor NdFeAsO1-xFx compound and a MnP-type FeAs phase, with dissimilar characteristic Raman bands. It was found that fluorine doping leads to structure disorder in the insulator Nd-O layers and high temperature coefficient of Fe-As vibrational mode.
We present results of transport and magnetic properties and heat capacity measurements on polycrystalline CeFeAsO, PrFeAsO, and NdFeAsO. These materials undergo structural phase transitions, spin density wave-like magnetic ordering of small moments on iron, and antiferromagnetic ordering of rare earth moments. The temperature dependence of the electrical resistivity, Seebeck coefficient, thermal conductivity, Hall coefficient, and magnetoresistance are reported. The magnetic behavior of the materials have been investigated using Mossbauer spectroscopy and magnetization measurements. Transport …
Single crystals of LaFeAsO, NdFeAsO, and SmFeAsO have been prepared by means of a NaAs flux growth technique and studied by optical spectroscopy measurements. We show that the spectral features corresponding to the partial energy gaps in the spin-density-wave (SDW) state are present below the structural phase transition. This indicates that the electronic state below the structural phase transition is already very close to that in the SDW state. We also show that in-plane infrared phonon modes display systematic shifts towards high frequency upon rare-earth element substitutions for La, sugges…
We have performed polarized Raman scattering measurements on the newly discovered superconductor Nd(O,F)BiS$_2$ ($T_c = 4$ K). We observe 2 Raman active modes, with frequencies in accordance with first-principles calculations. One A$_{1g}$ phonon mode at 112.4 cm$^{-1}$ exhibits a Fano line shape due to electron-phonon coupling. We find a resonance for this mode at 2.45 eV excitation energy. We estimate a 0.68 contribution of this mode to the electron-phonon coupling constant $λ$. Our Raman results suggest that the BiS$_2$-based superconductors are possibly phonon-mediated BCS superconductors.
Polarized Raman scattering measurements have been performed on Na0.5CoO2 single crystal from 8 to 305 K. Both the A1g and E1g phonon modes show a softening below Tc1 ~ 83 K. Additionally, the A1g phonon mode, which is forbidden in the scattering geometry of cross polarization for the triangular CoO2 layers, appears below Tc1. In contrast, the metal-insulator transition at Tc2 ~ 46 K has only secondary effect on the Raman spectra. The phonon softening and the ``forbidden'' Raman intensity follow closely magnetic order parameter and the gap function at the Fermi surface, indicating that the dist…
Temperature dependent Raman scattering studies in polycrystalline MgB2(10<T<300 K)reveal that the E2g phonon does not experience any self energy renormalization effect across the superconducting critical temperature Tc ~ 40 K. In contrast, most of the current theoretical models rely on the role of the E2g phonon in the electron-phonon coupling mechanism of superconductivity in MgB2. According to these models, a hardening of 12% is expected below Tc at the Gamma point of the Brillouim zone. In the presence of our results, those models must be reviewed. The analysis of the temperature dependence…
We report a Raman scattering study of nematic degrees of freedom in the iron-based superconductor parent compound BaFe$_2$As$_2$ under tunable uniaxial strain. We demonstrate that the polarization resolved arsenic (As) phonon intensity can be used to monitor the nematic order parameter as a function of both temperature and strain. At low temperature in the nematic ordered phase we use it to track the continuous and reversible orientation of nematic domains under variable strain. At higher temperature, the evolution of the As phonon intensity under strain reflects an enhanced nematic susceptibi…
We performed a polarized Raman scattering study of quasi-one-dimensional superconductor K$_2$Cr$_3$As$_3$. We detect two A$_1^\prime$ phonons and three E$^\prime$ phonons. One of the A$_1^\prime$ modes exhibits a nearly temperature-independent Fano lineshape. Based on our first-principles calculations, we ascribe this mode to the in-phase vibrations of Cr atoms within one layer. This observation strongly suggests that the magnetic fluctuations in K$_2$Cr$_3$As$_3$ are coupled to the electronic structure \emph{via} the lattice.
We determine the pressure dependence of the electron-phonon coupling constant in $κ$-(BEDT-TTF)$_{2}$Cu(SCN)$_{2}$ by comparison of high pressure Raman scattering and high pressure infrared reflectivity (IR) measurements. We use comparison of the IR reflection spectrum from deuterated and protonated samples to aid the deconvolution of several overlapping phonon modes. These coupled modes are modelled with a Green's function to extract the linear pressure dependence of the individual modes. The Raman active molecular vibrations of the BEDT-TTF dimers stiffen by 0.1-1 %GPa$^{-1}$. In contrast, t…
Recently discovered magnetic topological insulators $T$Bi$_{2}$Te$_{4}$ ($T=$Mn, Fe) crystallize into the $R\bar{3}m$ rhombohedral structure and exhibit the antiferromagnetic order. Here, we discuss the lattice dynamics of these compounds to confirm the stability of these systems. We show that the phonon dispersion does not contain soft modes, so both compounds are dynamically stable in the $R\bar{3}m$ phase. We perform theoretical analyses of the mode activity at $Γ$ point for the discussed compounds. In the case of the Raman active modes, our results are in agreement with the experimentally …
We present Raman measurements on the iron-pnictide superconductors CeFeAsO_{1-x}F_{x} and NdFeAsO{1-x}F_{x}. Modeling the Fe-As plane in terms of harmonic and a cubic anharmonic Fe-As interaction we calculate the temperature dependence of the energy and lifetime of the Raman active Fe B_{1g} mode and fit to the observed energy shift. The shifts and lifetimes are in good agreement with those measured also in other Raman studies which demonstrate that the phonon spectrum is well represented by phonon-phonon interactions without any significant electronic contribution. We also estimate the anharm…
We report the first systematic measurements of the Raman scattering by electrons in elemental metals of Al, Mo, Nb, Os, Pb, Re, Ta, Ti, V, W and metallic compound La$B_6$. Experimental spectra are modelled on the base of the band structures, calculated within the density functional theory, taking properly into account the effects of electron-phonon scattering. The agreement between our measured and calculated spectra is excellent for the variety of metals, thus providing estimates for the electron-phonon coupling constants and temperature-dependent relaxation rates. The method can be applied f…
The interplay between spin dynamics and lattice vibration has been suggested as an important part of the puzzle of high-temperature superconductivity. Here we report the strong interaction between spin fluctuation and phonon in SmFeAsO, a parent compound of the iron arsenide family of superconductors, revealed by low-temperature Raman spectroscopy. Anomalous zone-boundary-phonon Raman scattering from spin superstructure was observed at temperatures below the antiferromagnetic ordering point, which offers compelling evidence on spin dependent electron-phonon coupling in pnictides.
The paper presents detailed Raman scattering study of the unusually broad E2g phonon mode in MgB2 crystal. For the first time, it is shown by the polarized Raman scattering on few-micron-size crystallites with natural faces that the observed broad Raman feature really does obey the selection rules of an E2g mode. Raman spectra on high quality polycrystalline superconducting MgB2 wires reveal a very symmetric E2g phonon line near 615 1/cm with the room temperature linewidth of 260 1/cm only. Additional scattering of different polarization dependence, observed in certain crystallites is interpre…
We propose a microscopic theory of interaction of long wave molecular phonons with electrons in fullerides in the presence of disorder. Phonon relaxation rate and frequency renormalization are discussed. Finite electronic bandwidth reduces phonon relaxation rate at $q=0$. Electron-phonon coupling constants with molecular modes in fullerides are estimated. The results are in good agreement with photoemission experiments.
We argue that Raman scattering in $B_{1g}$ symmetry allows one to distinguish between phonon-mediated and magnetically-mediated $d-$wave superconductivity. In spin mediated superconductors, $B_{1g}$ Raman intensity develops a resonance at a frequency $ω_{res} < 2Δ_{max}$, whose origin is similar to a neutron resonance. In phonon-mediated $d-$wave superconductors, such a resonance does not develop. Several extensions of the argument are presented.
Electron-phonon coupling (EPC) is one of the most common and fundamental interactions in solids. It not only dominates many basic dynamic processes like resistivity, thermal conductivity etc, but also provides the pairing glue in conventional superconductors. But in high-temperature superconductors (HTSC), it is still controversial whether or not EPC is in favor of paring. Despite the controversies, many experiments have provided clear evidence for EPC in HTSC. In this paper, we briefly review EPC in cuprate and iron-based superconducting systems revealed by Raman scattering. We introduce how …
We report the polarized Raman spectra of undoped ReOFeAs (Re = Sm, La) collected at room temperature from $ab$ surfaces of impurity free microcrystals. The spectra exhibit sharp phonon lines on very weak electronic scattering background. The frequency and symmetry of the four Raman phonons involving out-of-plane atomic vibrations are found at 170 cm-1 (A1g, Sm), 201 cm-1 (A1g, As), 208 cm-1 (B1g, Fe), 345 cm-1(B1g, O) for SmOFeAs, and 162 cm-1 (A1g, La), 208 cm-1 (A1g, As), 201 cm-1 (B1g, Fe), 316 cm-1 (B1g, O) for LaOFeAs.
The anomalous features of the Raman spectroscopy measurement in MgB$_2$ represent a still unresolved puzzle. In particular highly debated are the origin of the huge $E_{2g}$ phonon linewidth, the nature of the low energy ($ω< ω_{E_{2g}}$) background and the evolution of the Raman spectra with Al doping. In this paper we compute the self-energy of the $E_{2g}$ phonon mode in a fully self-consistent way taking into account electron-phonon effects on the electronic properties. We show that all the anomalous features can be naturally understood in a framework where the whole electron-phonon spectr…
We performed a Raman scattering study of thin films of LiTi$_2$O$_4$ spinel oxide superconductor. We detected four out of five Raman active modes, with frequencies in good accordance with our first-principles calculations. Three T$_{2g}$ modes show a Fano lineshape from 5 K to 295 K, which suggests an electron-phonon coupling in LiTi$_2$O$_4$. Interestingly, the electron-phonon coupling shows an anomaly across the negative to positive magnetoresistance transition at 50 K, which may be due to the unset of other competing orders. The strength of the electron-phonon interaction estimated from the…
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…
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…
We use polarization-resolved Raman scattering to study lattice dynamics in NaFe$_{0.53}$Cu$_{0.47}$As single crystals. We identify 4 $A_{1g}$ phonon modes at 125, 172, 183 and 197 cm$^{-1}$, and 4 $B_{3g}$ phonon modes at 101, 138, 173, 226 cm$^{-1}$. The phonon spectra are consistent with the $Ibam$ group, which confirms that the Cu and Fe atoms form a stripe order. The temperature dependence of the phonon spectra suggests weak electron-phonon and magneto-elastic interactions.
The effect of pressure on optical phonon frequencies of MgB$_2$ has been calculated using the frozen-phonon approach based on a pseudopotential method. Grüneisen parameters of the harmonic mode frequencies are reported for the high-frequency zone-center $E_{2g}$ and $B_{1g}$ and the zone-boundary $E_{2u}$ and $B_{2u}$ modes at $A$. Anharmonic effects of phonon frequencies and the implications of the calculated phonon frequency shifts for the pressure dependence of the superconducting transition temperature of MgB$_2$ are discussed. Also reported are Raman and optical reflectance spectra of MgB…
We consider a model Hamiltonian fitted on the ab-initio band structure to describe the electron-phonon coupling between the electronic $σ-$bands and the phonon E$_{2g}$ mode in MgB$_2$. The model allows for analytical calculations and numerical treatments using very large k-point grids. We calculate the phonon self-energy of the E$_{2g}$ mode along two high symmetry directions in the Brillouin zone. We demonstrate that the contribution of the $σ$ bands to the Raman linewidth of the E$_{2g}$ mode via the electron-phonon coupling is zero. As a consequence the large resonance seen in Raman experi…
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 …
Time resolved measurements provide a new way to disentangle complex interactions in quantum materials due to their different timescales. We used pump-probe Raman scattering to investigate the apical oxygen vibration in YBa$_2$Cu$_3$O$_{6+x}$ under nonequilibrium conditions. Time-dependence of the phonon population demonstrated strong electron-phonon coupling. Most importantly, the phonon shifts to a higher energy due to transient smearing of the Fermi surface in a remarkable agreement with diagrammatic theory. We also discuss new insights into photoinduced superconductivity reported at lower d…
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…
The two-loop temperature hysteresis of integrated intensity of Raman scattering of light is explained theoretically for a line of frequency 50 cm-1 in a superconducting oxide Ba1-xKxBiO3 single crystal.
We present a theoretical ab-initio approach that allows us to explicitly calculate the superconducting transition temperatures (Tc) of the iron-based superconductors of LaFeAsO1-xFx, SmFeAsO1-xFx, NdFeAsO1-xFx, Ba1-xKxFe2As2, FeSe and LiFeAs that fit perfectly with the experiments. We consider recent evidence that electron-phonon coupling may have been underestimated previously, and a prediction that antiferromagnetism can greatly enhance electron-phonon coupling through localized iron d orbitals. We then include the contribution of these localized orbitals in a McMillan formalism. In addition…
We report temperature-dependent Raman spectra of CeFeAsO0.9F0.1 from 4 K to 300 K in spectral range of 60 to 1800 cm-1 and interpret them using estimates of phonon frequencies obtained from first-principles density functional calculations. We find evidence for a strong coupling between the phonons and crystal field excitations; in particular Ce3+ crystal field excitation at 432 cm-1 couples strongly with Eg oxygen vibration at 389 cm-1 . Below the superconducting transition temperature, the phonon mode near 280 cm-1 shows softening, signaling its coupling with the superconducting gap. The rati…
We have measured Raman scattering spectra of single-crystalline FeTe0.6Se0.4 (T_c ~ 14.5 K) and its parent compound Fe1.074Te at various temperatures. In the parent compound Fe1.074Te, A1g and B1g modes have been observed at 157.5 and 202.3 cm-1, respectively, at 5 K. These frequencies qualitatively agree with the calculated results. Two-magnon excitation has been observed around 2300 cm-1 for both compounds. Temperature dependence between the electronic Raman spectra below and above T_c has been observed and 2Δand 2Δ/k_BT_C have been estimated as 5.0 meV and 4.0, respectively.
The Raman spectrum of the superconductor MgB$_{2}$ has been measured as a function of the Tc of the film. A striking correlation is observed between the $T_{c}$ onset and the frequency of the $E_{2g}$ mode. Analysis of the data with the McMillan formula provides clear experimental evidence for the collapse of the electron phonon coupling at the temperature predicted for the convergence of two superconducting gaps into one observable gap. This gives indirect evidence of the convergence of the two gaps and direct evidence of a transition to an isotropic state at 19 K. The value of the electron p…
Interference-Enhanced Large Electron-Phonon Coupling from Raman-active Breathing Modes in Moiré Semiconductors
Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Shanghai Jiao Tong University（上海交通大学）；National Institute for Materials Science（物质材料研究机构）；University of Tennessee（田纳西大学）
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…
Room temperature Raman scattering measurements have been carried out on well characterized samples of MgB2-xCx. The Raman line corresponding to the E2g phonon mode shows progressive hardening from 620 cm-1 in pristine MgB2 to 775 cm-1 in the sample with carbon fraction x=0.2. The corresponding line width on the other hand, increases from a value of about 220 cm-1 to 286 cm-1 in samples with x = 0.1, beyond which it decreases to a value 167 cm-1 for x=0.2. From the average mode frequency and the line width obtained from Raman measurements and taking the values of N(0) obtained from the calculat…
The polarized Raman spectra from ab and ac surfaces of single crystal NaxCoO2 (x~0.7), parent compound of recently discovered superconductor NaxCoO2.yH2O, are reported and discussed. The crystals were hexagon platelets of typical size 3x3x0.1 mm. Three of the five (A1g+E1g+3E2g) Raman active phonons were unambiguously identified at 458 (E1g), 494(E2g) and 574 (A1g) cm-1. The spectra from ab and ac surfaces differ significantly and provide evidence that within hours after preparation the ac surface, unlike the ab one, is strongly disordered. Within several days the disorder extends over the ab …
