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We studied the electronic Raman spectra of (Li$_{1-x}$Fe$_x$)OHFeSe as a function of light polarization and temperature. In the B$_{1g}$ spectra alone we observe the redistribution of spectral weight expected for a superconductor and two well-resolved peaks below T$_c$. The nearly resolution-limited peak at 110 cm$^{-1}$ (13.6 meV) is identified as a collective mode. The peak at 190 cm$^{-1}$ (23.6 meV) is presumably another collective mode since the line is symmetric and its energy is significantly below the gap energy observed by single-particle spectroscopies. Given the experimental band structure of (Li$_{1-x}$Fe$_x$)OHFeSe, the most plausible explanations include conventional spin-fluctuation pairing between the electron bands and the incipient hole band and pairing between the hybridized electron bands. The absence of gap features in A$_{1g}$ and B$_{2g}$ symmetry favors the second case. Thus, in spite of various differences between the pnictides and chalcogenides, this Letter demonstrates the proximity of pairing states and the importance of band structure effects in the Fe-based compounds., Comment: 9 pages, 12 figures

Connections between crystal chemistry and critical temperature $T_c$ have been in the focus of superconductivity, one of the most widely studied phenomena in physics, chemistry and materials science alike. In most Fe-based superconductors, materials chemistry and physics conspire so that $T_c$ correlates with the average anion height above the Fe plane, i. e. with the geometry of the FeAs4 or FeCh4 (Ch = Te, Se, or S) tetrahedron. By synthesizing Fe$_{1-y}$Se$_{1-x}$S$_x$ (0$\leq$$x$$\leq$1, $y$$\leq$0.1), we find that in alloyed crystals $T_c$ is not correlated with the anion height like it is for most other Fe superconductors. Instead, changes in $T_c$($x$) and tetragonal-to-orthorombic (nematic) transition $T_s$($x$) upon cooling are correlated with disorder in Fe vibrations in the direction orthogonal to Fe planes, along the crystallographic c-axis. The disorder stems from the random nature of S substitution, causing deformed Fe(Se,S)4 tetrahedra with different Fe-Se and Fe-S bond distances. Our results provide evidence of $T_c$ and $T_s$ suppression by disorder in anion height. The connection to local crystal chemistry may be exploited in computational prediction of new superconducting materials with Fe/S building blocks., Comment: 10 pages, 5 figures

We report inelastic light scattering results on the stoichiometric and fully ordered superconductor CaKFe$_4$As$_2$ as a function of temperature and light polarization. In the energy range between 10 and 315 cm$^{-1}$ (1.24 and 39.1 meV) we observe the particle-hole continuum above and below the superconducting transition temperature $T_c$ and 7 of the 8 Raman active phonons. The main focus is placed on the analysis of the electronic excitations. Below $T_c$ all three symmetries projected with in-plane polarizations display a redistribution of spectral weight characteristic for superconductivity. The energies of the pair-breaking peaks in $A_{1g}$ and $B_{2g}$ symmetry are in approximate agreement with the results from photoemission studies. In $B_{1g}$ symmetry the difference between normal and superconducting state is most pronounced, and the feature is shifted downwards with respect to those in $A_{1g}$ and $B_{2g}$ symmetry. The maximum peaking at 134 cm$^{-1}$ (16.6 meV) has a substructure on the high-energy side. We interpret the peak at 134 cm$^{-1}$ in terms of a collective Bardasis-Schrieffer (BS) mode and the substructure as a remainder of the pair-breaking feature on the electron bands. There is a very weak peak at 50 cm$^{-1}$ (6.2 meV) which is tentatively assigned to another BS mode., Comment: 8 pages, 9 figures

Resolving the microscopic pairing mechanism and its experimental identification in unconventional superconductors is among the most vexing problems of contemporary condensed matter physics. We show that Raman spectroscopy provides an avenue for this quest by probing the structure of the pairing interaction at play in an unconventional superconductor. As we study the spectra of the prototypical Fe-based superconductor ${\rm Ba_{1-x}K_xFe_2As_2}$ for $0.22\le x \le 0.70$ in all symmetry channels, Raman spectroscopy allows us to distill the leading $s$-wave state. In addition, the spectra collected in the $B_{1g}$ symmetry channel reveal the existence of two collective modes which are indicative of the presence of two competing, yet sub-dominant, pairing tendencies of $d_{x^2-y^2}$ symmetry type. A comprehensive functional Renormalization Group (fRG) and random-phase approximation (RPA) study on this compound confirms the presence of the two sub-leading channels, and consistently matches the experimental doping dependence of the related modes. The synopsis of experimental evidence and theoretical modelling supports a spin-fluctuation mediated superconducting pairing mechanism., Comment: 13 pages, 13 figures

For carbon nanotubes filled with fullerenes ("peapods"), it is a key issue to find an analytical method that distinguishes the molecules inside the nanotube from those adsorbed on its surface. High resolution transmission electron microscopy (HRTEM) detects both encapsulated and adsorbed molecules which are large enough (e.g., fullerenes), but being a localprobe method, it cannot be applied to large amounts of sample. In Raman spectroscopy, the empirical rules for line shifts and splitting are nanotube-type dependent and often ambiguous. We prepared C-60 peapods by nano-extraction using supercritical CO2 as a solvent, and subsequently removed the adsorbed fulkrene molecules by washing the samples. We analyzed the samples by the combination of HRTEM, Raman, and midinfrared attenuated total reflectance (MIR-) spectroscopy. Although the TEM images proved that the nanotubes were filled with fullerenes, we did not observe any shift in the fullerene's A(g)(2) Raman mode compared to C-60 crystals. ATR spectra, on the other hand, were found to detect only the adsorbed molecules. Therefore, the combination of the two methods provide good basis for determining the success of nanotube filling by spectroscopy alone. Refereed/Peer-reviewed

Non-covalent functionalization of carbon nanotubes (CNTs) by polymers or aromatic systems is a rapidly emerging field. Its importance originates in the possibility of combining special (optical, electric, or dispersive) properties of the added molecules with the mechanical stability of nanotubes. A special application is to use the polymers as interfaces between nanotubes and metallic nanoparticles ("molecular glue"). Crucial to all applications is an experimental tool to characterize the interaction strength between the nanotubes and the associated species. In this paper, we study hybrids of single-walled nanotubes (SWNT) and polyallylamine obtained from poly(allylamine hydrochloride) (PAH) at high pH. We use attenuated total reflection (ATR) spectroscopy and Raman spectroscopy to understand how polyallylamine covers the surface of the nanotubes. The interaction of the evanescent field on the surface of the nanotube with the vibrations of the adsorbed species invokes surface selection rules and, hence, surface-attenuated infrared absorption (SAIRA). Raman spectra prove diameter-selective solubilization of the polymer-covered nanotubes. Refereed/Peer-reviewed

By exposing flat and curved carbon surfaces to coronene, a variety of van der Waals hybrid heterostructures are prepared, including coronene encapsulated in carbon nanotubes, and coronene and dicoronylene adsorbed on nanotubes or graphite via - interactions. The structure of the final product is determined by the temperature of the experiment and the curvature of the carbon surface. While at temperatures below and close to the sublimation point of coronene, nanotubes with suitable diameters are filled with single coronene molecules, at higher temperatures additional dimerization and oligomerization of coronene occurs on the surface of carbon nanotubes. The fact that dicoronylene and possible higher oligomers are formed at lower temperatures than expected for vapor-phase polymerization indicates the active role of the carbon surface used primarily as template. Removal of adsorbed species from the nanotube surface is of utmost importance for reliable characterization of encapsulated molecules: it is demonstrated that the green fluorescence attributed previously to encapsulated coronene is instead caused by dicoronylene adsorbed on the surface which can be solubilized and removed using surfactants. After removing most of the adsorbed layer, a combination of Raman spectroscopy and transmission electron microscopy was employed to follow the transformation dynamics of coronene molecules inside nanotubes. Refereed/Peer-reviewed