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Register a new userHigh Resolution Photoemission Study on Low-T_K Ce Systems: Kondo Resonance, Crystal Field Structures, and their Temperature Dependence
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We present a high-resolution photoemission study on the strongly correlated Ce-compounds CeCu_6, CeCu_2Si_2, CeRu_2Si_2, CeNi_2Ge_2, and CeSi_2. Using a normalization procedure based on a division by the Fermi-Dirac distribution we get access to the spectral density of states up to an energy of 5 k_BT above the Fermi energy E_F. Thus we can resolve the Kondo resonance and the crystal field (CF) fine-structure for different temperatures above and around the Kondo temperature T_K. The CF peaks are identified with multiple Kondo resonances within the multiorbital Anderson impurity model. Our theoretical 4f spectra, calculated from an extended non-crossing approximation (NCA), describe consistently the observed photoemission features and their temperature dependence. By fitting the NCA spectra to the experimental data and extrapolating the former to low temperatures, T_K can be extracted quantitatively. The resulting values for T_K and the crystal field energies are in excellent agreement with the results from bulk sensitive measurements, e.g. inelastic neutron scattering.
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Resonant photoemission (RPES) at the Ce 3d -> 4f threshold has been performed for alpha-like compound CeNi_2 with extremely high energy resolution (full width at half maximum < 0.2 eV) to obtain bulk-sensitive 4f spectral weight. The on-resonance spectrum shows a sharp resolution-limited peak near the Fermi energy which can be assigned to the tail of the Kondo resonance. However, the spin-orbit side band around 0.3 eV binding energy corresponding to the f_{7/2} peak is washed out, in contrast to the RPES spectrum at the Ce 3d -> 4f RPES threshold. This is interpreted as due to the different surface sensitivity, and the bulk-sensitive Ce 3d -> 4f RPES spectra are found to be consistent with other electron spectroscopy and low energy properties for alpha-like Ce-transition metal compounds, thus resolves controversy on the interpretation of Ce compound photoemission. The 4f spectral weight over the whole valence band can also be fitted fairly well with the Gunnarsson-Schoenhammer calculation of the single impurity Anderson model, although the detailed features show some dependence on the hybridization band shape and (possibly) Ce 5d emissions.
We calculate the Kondo temperature ($T_K$) and crystal-field levels of strongly correlated multiorbital systems solving the Anderson Impurity Model with the finite U Non-Crossing Approximation (UNCA) in its simplest scheme, that is, considering the self energies at lowest order in the 1/N diagrammatic expansion. We introduced an approximation to the vertex function that includes the double energy dependence and investigate its effect on the values of $T_K$ for simple electronic models. We also analyze the competition between the two spin flip mechanisms, involving virtual transitions to empty and doubly occupied states, in the determination of the ground state symmetry by including an extra diagram of higher order in $1/N.$ We finally combine the resulting simple formalism with {it ab initio} calculated electronic structures to obtain $T_K$s, ground states, and crystal field splittings in excellent agreement with experimental results for two particular Ce compounds, namely CeIn$_3$ and CeSn$_3$.
Spin- and angle-resolved resonant (Ce $4dto4f$) photoemission spectra of a monolayer Ce on Fe(110) reveal spin-dependent changes of the Fermi-level peak intensities. That indicate a spin-dependence of $4f$ hybridization and, thus, of $4f$ occupancy and local moment. The phenomenon is described in the framework of the periodic Anderson model by $4f$ electron hopping into the exchange split Fe 3d derived bands that form a spin-gap at the Fermi energy around the $bar{Gamma}$ point of the surface Brillouin zone.
We present high-resolution photoemission spectroscopy studies on the Kondo resonance of the strongly-correlated Ce system CeCu$_2$Si$_2$. Exploiting the thermal broadening of the Fermi edge we analyze position, spectral weight, and temperature dependence of the low-energy 4f spectral features, whose major weight lies above the Fermi level $E_F$. We also present theoretical predictions based on the single-impurity Anderson model using an extended non-crossing approximation (NCA), including all spin-orbit and crystal field splittings of the 4f states. The excellent agreement between theory and experiment provides strong evidence that the spectral properties of CeCu$_2$Si$_2$ can be described by single-impurity Kondo physics down to $T approx 5$ K.
The bulk-sensitive Ce 4$f$ spectral weights of various Ce compounds including CeFe$_2$, CeNi$_2$, and CeSi$_2$ were obtained with the resonant photoemission technique at the Ce 3d-edge. We found the lineshapes change significantly with the small change of the incident photon energy. Detailed analysis showed that this phenomenon results primarily from the Auger transition between different multiplet states of the Ce $underline{3d_{5/2}}4f^2$ (bar denotes a hole) electronic configuration in the intermediate state of the resonant process. This tells us that extra care should be taken for the choice of the resonant photon energy when extracting Ce 4$f$ spectral weights from the Ce 3$d$-edge resonant photoemission spectra. The absorption energy corresponding to the lowest multiplet structure of the Ce $underline{3d_{5/2}}4f^2$ configuration seems to be the logical choice.
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