Electronic properties of correlated metals in the vicinity of a charge order transition: optical spectroscopy of α\alpha-(BEDT-TTF)2M_2MHg(SCN)4_4 (MM = NH4_4, Rb, Tl)

The infrared spectra of the quasi-two-dimensional organic conductors $\alpha$-(BEDT-TTF)$_2$$M$Hg(SCN)$_4$ ($M$ = NH$_4$, Rb, Tl) were measured in the range from 50 to 7000 \cm down to low temperatures in order to explore the influence of electronic correlations in quarter-filled metals. The interpretation of electronic spectra was confirmed by measurements of pressure dependant reflectance of $\alpha$-(BEDT-TTF)$_2$KHg(SCN)$_4$ at T=300 K. The signatures of charge order fluctuations become more pronounced when going from the NH$_4$ salt to Rb and further to Tl compounds. On reducing the temperature, the metallic character of the optical response in the NH$_4$ and Rb salts increases, and the effective mass diminishes. For the Tl compound, clear signatures of charge order are found albeit the metallic properties still dominate. From the temperature dependence of the electronic scattering rate the crossover temperature is estimated below which the coherent charge-carriers response sets in. The observations are in excellent agreement with recent theoretical predictions for a quarter-filled metallic system close to charge order

Zero temperature optical conductivity of ultra-clean Fermi liquids and superconductors

We calculate the low-frequency optical conductivity sigma(w) of clean metals and superconductors at zero temperature neglecting the effects of impurities and phonons. In general, the frequency and temperature dependences of sigma have very little in common. For small Fermi surfaces in three dimensions (but not in 2D) we find for example that Re sigma(w>0)=const. for low w which corresponds to a scattering rate Gamma proportional to w^2 even in the absence of Umklapp scattering when there is no T^2 contribution to Gamma. In the main part of the paper we discuss in detail the optical conductivity of d-wave superconductors in 2D where Re sigma(w>0) \propto w^4 for the smallest frequencies and the Umklapp processes typically set in smoothly above a finite threshold w_0 smaller than twice the maximal gap Delta. In cases where the nodes are located at (pi/2, pi/2), such that direct Umklapp scattering among them is possible, one obtains Re sigma(w) \propto w^2.Comment: 7 pages, 3 figure

Competition between Charge Ordering and Superconductivity in Layered Organic Conductors α\alpha-(BEDT-TTF)2M_2MHg(SCN)4_4 (M = K, NH4_4)

While the optical properties of the superconducting salt $\alpha$-(BEDT-TTF)$_2$NH$_4$Hg(SCN)$_4$ remain metallic down to 2 K, in the non-superconducting K-analog a pseudogap develops at frequencies of about 200 cm$^{-1}$ for temperatures T < 200 K. Based on exact diagonalisation calculations on an extended Hubbard model at quarter-filling we argue that fluctuations associated with short range charge ordering are responsible for the observed low-frequency feature. The different ground states, including superconductivity, are a consequence of the proximity of these compounds to a quantum phase charge-ordering transition driven by the intermolecular Coulomb repulsion.Comment: 4 pages, 3 figure

Pressure-dependent optical investigations of α\alpha-(BEDT-TTF)2_2I3_3: tuning charge order and narrow gap towards a Dirac semimetal

Infrared optical investigations of $\alpha$-(BEDT-TTF)$_2$I$_3$ have been performed in the spectral range from 80 to 8000~cm$^{-1}$ down to temperatures as low as 10~K by applying hydrostatic pressure. In the metallic state, $T > 135$~K, we observe a 50\% increase in the Drude contribution as well as the mid-infrared band due to the growing intermolecular orbital overlap with pressure up to 11~kbar. In the ordered state, $T<T_{\rm CO}$, we extract how the electronic charge per molecule varies with temperature and pressure: Transport and optical studies demonstrate that charge order and metal-insulator transition coincide and consistently yield a linear decrease of the transition temperature $T_{\rm CO}$ by $8-9$~K/kbar. The charge disproportionation $\Delta\rho$ diminishes by $0.017~e$/kbar and the optical gap $\Delta$ between the bands decreases with pressure by -47~cm$^{-1}$/kbar. In our high-pressure and low-temperature experiments, we do observe contributions from the massive charge carriers as well as from massless Dirac electrons to the low-frequency optical conductivity, however, without being able to disentangle them unambiguously.Comment: 13 pages, 17 figures, submitted to Phys. Rev.

Signatures of electron-boson coupling in half-metallic ferromagnet Mn5_5Ge3_3: study of electron self-energy Σ(ω)\Sigma(\omega) obtained from infrared spectroscopy

We report results of our infrared and optical spectroscopy study of a half-metallic ferromagnet Mn$_5$Ge$_3$. This compound is currently being investigated as a potential injector of spin polarized currents into germanium. Infrared measurements have been performed over a broad frequency (50 - 50000 cm$^{-1}$) and temperature (10 - 300 K) range. From the complex optical conductivity $\sigma(\omega)$ we extract the electron self-energy $\Sigma(\omega)$. The calculation of $\Sigma(\omega)$ is based on novel numerical algorithms for solution of systems of non-linear equations. The obtained self-energy provides a new insight into electron correlations in Mn$_5$Ge$_3$. In particular, it reveals that charge carriers may be coupled to bosonic modes, possibly of magnetic origin

Enhancement of Wigner crystallization in quasi low-dimensional solids

The crystallization of electrons in quasi low-dimensional solids is studied in a model which retains the full three-dimensional nature of the Coulomb interactions. We show that restricting the electron motion to layers (or chains) gives rise to a rich sequence of structural transitions upon varying the particle density. In addition, the concurrence of low-dimensional electron motion and isotropic Coulomb interactions leads to a sizeable stabilization of the Wigner crystal, which could be one of the mechanisms at the origin of the charge ordered phases frequently observed in such compounds

Optical properties of the Ce and La di-telluride charge density wave compounds

The La and Ce di-tellurides LaTe$_2$ and CeTe$_2$ are deep in the charge-density-wave (CDW) ground state even at 300 K. We have collected their electrodynamic response over a broad spectral range from the far infrared up to the ultraviolet. We establish the energy scale of the single particle excitation across the CDW gap. Moreover, we find that the CDW collective state gaps a very large portion of the Fermi surface. Similarly to the related rare earth tri-tellurides, we envisage that interactions and Umklapp processes play a role in the onset of the CDW broken symmetry ground state