Formation of metallic magnetic clusters in a Kondo-lattice metal: Evidence from an optical study

Magnetic materials are usually divided into two classes: those with localised magnetic moments, and those with itinerant charge carriers. We present a comprehensive experimental (spectroscopic ellipsomerty) and theoretical study to demonstrate that these two types of magnetism do not only coexist but complement each other in the Kondo-lattice metal, Tb2PdSi3. In this material the itinerant charge carriers interact with large localised magnetic moments of Tb(4f) states, forming complex magnetic lattices at low temperatures, which we associate with self-organisation of magnetic clusters. The formation of magnetic clusters results in low-energy optical spectral weight shifts, which correspond to opening of the pseudogap in the conduction band of the itinerant charge carriers and development of the low- and high-spin intersite electronic transitions. This phenomenon, driven by self-trapping of electrons by magnetic fluctuations, could be common in correlated metals, including besides Kondo-lattice metals, Fe-based and cuprate superconductors

Low energy Mott Hubbard excitations in LaMnO3 probed by optical ellipsometry

We present a comprehensive ellipsometric study of an untwinned, nearly stoichiometric LaMnO 3 crystal in the spectral range 1.2–6.0 eV at temperatures 20≤T≤300 K . The complex dielectric response along b and c axes of the Pbnm orthorhombic unit cell, ε ̃ b (ν) and ε ̃ c (ν) , is highly anisotropic over the spectral range covered in the experiment. The difference between ε ̃ b (ν) and ε ̃ c (ν) increases with decreasing temperature, and the gradual evolution observed in the paramagnetic state is strongly enhanced by the onset of A -type antiferromagnetic long-range order at T N =139.6 K . In this study we focus on the analysis of excitations observed at high energy (∼4–5 eV) and show that the observed temperature changes of their spectral weight are opposite to those found for the lowest-energy gap excitation at ∼2 eV . We used a classical dispersion analysis to quantitatively determine the temperature-dependent optical spectral-weights shifts between low- and high-energy optical bands. Based on the observation of a pronounced spectral-weight transfer between both features upon magnetic ordering, they are assigned to high-spin and low-spin intersite d 4 d 4 ⇌d 3 d 5 transitions by Mn electrons. The anisotropy of the lowest-energy optical band and the spectral-weight shifts induced by antiferromagnetic spin correlations are quantitatively described by an effective spin-orbital superexchange model. An analysis of the multiplet structure of the intersite transitions by Mn e g electrons allowed us to estimate the effective intra-atomic Coulomb interaction, the Hund exchange coupling, and the Jahn-Teller splitting energy between e g orbitals in LaMnO 3 , as well as to extract experimental information concerning the type of orbital order in LaMnO 3 . This study identifies the lowest-energy optical transition at ∼2 eV as an intersite d-d transition whose energy is substantially reduced compared to that obtained from the bare intra-atomic Coulomb interaction

Optical investigation of LaMnO 3 thin films: a study of the 2-eV band

We measure the transmittance of LaMnO 3 (LMO) thin films in the spectral range from 10 000 to 38 000 cm -1 as a function of temperature. The optical conductivity obtained from the transmittance data is decomposed into five Drude-Lorentz contributions: three of them show evident changes below the Néel temperature T N $\simeq$ 140 K. We discuss the band assignment in the framework of the tight-binding and of the orbitally degenerate Hubbard models. Our results ascribe the overall low-frequency spectrum of LMO to charge-transfer mechanisms involving the t 2g and e g electrons of the Mn ions, without invoking the presence of excitonic contributions. This finding definitely promotes a Mott-Hubbard scenario for LMO and provides an estimate of the Hamiltonian parameters. Copyright EDP Sciences, SIF, Springer-Verlag Berlin Heidelberg 2011