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Register a new userThermodynamics of the $alpha$-$gamma$ transition in cerium studied by an LDA + Gutzwiller method
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The $alpha$-$gamma$ transition in cerium has been studied in both zero and finite temperature by Gutzwiller density functional theory. We find that the first order transition between $alpha$ and $gamma$ phases persists to the zero temperature with negative pressure. By further including the entropy contributed by both electronic quasi-particles and lattice vibration, we obtain the total free energy at given volume and temperature, from which we obtain the $alpha$-$gamma$ transition from the first principle calculation. We also computed the phase diagram and pressure versus volume isotherms of cerium at finite temperature and pressure, finding excellent agreement with the experiments. Our calculation indicate that both the electronic entropy and lattice vibration entropy plays important role in the $alpha$-$gamma$ transition.
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We emphasize, on the basis of experimental data and theoretical calculations, that the entropic stabilization of the gamma-phase is the main driving force of the alpha-gamma transition of cerium in a wide temperature range below the critical point. Using a formulation of the total energy as a functional of the local density and of the f-orbital local Greens functions, we perform dynamical mean-field theory calculations within a new implementation based on the multiple LMTO method, which allows to include semi-core states. Our results are consistent with the experimental energy differences and with the qualitative picture of an entropy-driven transition, while also confirming the appearance of a stabilization energy of the alpha phase as the quasiparticle Kondo resonance develops.
Combining the density functional theory (DFT) and the Gutzwiller variational approach, a LDA+Gutzwiller method is developed to treat the correlated electron systems from {it ab-initio}. All variational parameters are self-consistently determined from total energy minimization. The method is computationally cheaper, yet the quasi-particle spectrum is well described through kinetic energy renormalization. It can be applied equally to the systems from weakly correlated metals to strongly correlated insulators. The calculated results for SrVO$_3$, Fe, Ni and NiO, show dramatic improvement over LDA and LDA+U.
We introduce in detail our newly developed textit{ab initio} LDA+Gutzwiller method, in which the Gutzwiller variational approach is naturally incorporated with the density functional theory (DFT) through the Gutzwiller density functional theory (GDFT) (which is a generalization of original Kohn-Sham formalism). This method can be used for ground state determination of electron systems ranging from weakly correlated metal to strongly correlated insulators with long-range ordering. We will show that its quality for ground state is as high as that by dynamic mean field theory (DMFT), and yet it is computationally much cheaper. In additions, the method is fully variational, the charge-density self-consistency can be naturally achieved, and the quantities, such as total energy, linear response, can be accurately obtained similar to LDA-type calculations. Applications on several typical systems are presented, and the characteristic aspects of this new method are clarified. The obtained results using LDA+Gutzwiller are in better agreement with existing experiments, suggesting significant improvements over LDA or LDA+U.
The $gamma to alpha$ isostructural transition in the Ce$_{0.9-x}$La$_x$Th$_{0.1}$ system is measured as a function of La alloying using specific heat, magnetic susceptibility, resistivity, thermal expansivity/striction measurements. A line of discontinuous transitions, as indicated by the change in volume, decreases exponentially from 118 K to close to zero with increasing La doping and the transition changes from being first-order to continuous at a critical concentration $0.10 leq x_c leq 0.14$. At the tricritical point, the coefficient of the linear $T$ term in the specific heat $gamma$ and the magnetic susceptibility start to increase rapidly near $x$ = 0.14 and gradually approaches large values at $x$=0.35 signifying that a heavy Fermi-liquid state evolves at large doping. Near $x_c$, the Wilson ratio, $R_W$, has a value of 3.0, signifying the presence of magnetic fluctuations. Also, the low-temperature resistivity shows that the character of the low-temperature Fermi-liquid is changing.
The ground states of Na$_x$CoO$_2$ ($0.0<x<1.0$) is studied by the LDA+Gutzwiller approach, where charge transfer and orbital fluctuations are all self-consistently treated {it ab-initio}. In contrast to previous studies, which are parameter-dependent, we characterized the phase diagram as: (1) Stoner magnetic metal for $x>0.6$ due to $a_{1g}$ van-Hove singularity near band top; (2) correlated non-magnetic metal without $e_g^{prime}$ pockets for $0.3<x<0.6$; (3) $e_g^{prime}$ pockets appear for $x<0.3$, and additional magnetic instability involves. Experimental quasi-particle properties is well explained, and the $a_{1g}$-$e_g^{prime}$ anti-crossing is attributed to spin-orbital coupling.
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