Добірка наукової літератури з теми "Density functional theory, RPA, beyond RPA, ACFDT"

The connection between the adiabatic excitation energy of time-dependent density functional theory and the ground state correlation energy from the adiabatic connection fluctuation–dissipation theorem (ACFDT) is explored in the limiting case of one excited state. An exact expression is derived for any adiabatic Hartree-exchange–correlation kernel that connects the excitation energy and the potential contribution to correlation. The resulting formula is applied to the asymmetric Hubbard dimer, a system where this limit is exact. Results from a hierarchy of approximations to the kernel, including the random phase approximation (RPA) with and without exchange and the adiabatically exact (AE) approximation, are compared to the exact ones. At full coupling, the numerical results indicate a tension between predicting an accurate excitation energy and an accurate potential contribution to correlation. The AE approximation is capable of making accurate predictions of both quantities, but only in parts of the parameter space that classify as weakly correlated, while RPA tends to be unable to accurately predict these properties simultaneously anywhere. For a strongly correlated dimer, the AE approximation greatly overestimates the excitation energy yet continues to yield an accurate ground state correlation energy due to its accurate prediction of the adiabatic connection integrand. If similar trends hold for real systems, the development of correlation kernels will be important for applications of the ACFDT in systems with large potential contributions to correlation.

Over time, many different theories and approaches have been developed to tackle the many-body problem in quantum chemistry, condensed-matter physics, and nuclear physics. Here we use the helium atom, a real system rather than a model, and we use the exact solution of its Schrödinger equation as a benchmark for comparison between methods. We present new results beyond the random-phase approximation (RPA) from a renormalized RPA (r-RPA) in the framework of the self-consistent RPA (SCRPA) originally developed in nuclear physics, and compare them with various other approaches like configuration interaction (CI), quantum Monte Carlo (QMC), time-dependent density-functional theory (TDDFT), and the Bethe-Salpeter equation on top of the \boldsymbol{GW}𝐆𝐖 approximation. Most of the calculations are consistently done on the same footing, e.g. using the same basis set, in an effort for a most faithful comparison between methods.

Density functional theory (DFT) within standard local density/generalized gradient approximations (LDA/GGAs) have been proved to succesfully predict the properties of a wide class of electronic systems at a reasonable computational time. However there exist a number of situations in wich DFT within LDA/GGAs qualitatively fails. One of such problems is their inability, due their intrinsic local nature, to describe long-range interaction between non overlapping molecular fragments, or weakly bound systems such as molecules about to break during a chemical reaction. The Adiabatic Connection Fluctuation Dissipation (ACFD) formalism tackle this kind of problems at a very foundamental level providing a perfect starting point for the development of truly non-local functionals. We have indeed developed and implemented an efficient scheme for the calculation of the correlation energy via the ACFD theorem going beyond the random phase approximation (RPA) by including the exact-exchange contribution to the kernel. We found that this contribution plays a crucial role for a correct and accurate description of the total energy of an electronic system without compromising the achivements of the original RPA functional.

Mean-field approaches successfully reproduce nuclear bulk properties like masses and radii within the Energy Density Functional (EDF) framework. However, complex correlations are missing in mean-field models and several observables related to single-particle and collective nuclear properties cannot be predicted accurately. The necessity to provide a precise description of the available data as well as reliable predictions in the exotic regions of the nuclear chart motivates the use of more sophisticated beyond-mean-field models. Correlations and higher-order corrections (beyond the leading mean-field order) are introduced. A crucial aspect in these calculations is the choice of the effective interaction to be used when one goes beyond the leading order (available effective interactions are commonly adjusted at the mean-field level). In the first part, we deal with the equation of state of nuclear matter evaluated up to the second order with the phenomenological Skyrme force. We analyze the ultraviolet divergence that is related to the zero range of the interaction and we introduce Skyrme-type regularized interactions that can be used at second order for matter. Cutoff regularization and dimen- sional regularization techniques are explored and applied. In the latter case, connections are naturally established between the EDF framework and some techniques employed in Effective Field Theories. In the second part, we check whether the regularized interactions introduced for nuclear matter can be employed also for finite nuclei. As an illustration, this analysis is performed within the particle- vibration model that represents an example of beyond mean-field models where an ultraviolet divergence appears if zero-range forces are used. These first applications suggest several directions to be explored to finally provide regularized interactions that are specially tailored for beyond- mean-field calculations for finite nuclei. Conclusions and perspectives are finally illustrated.

Density Functional Theory is one of the most widely used methods in quantum calculations of the electronic structure of matter in both condensed matter physics and quantum chemistry. Despite the importance of the density functional theory to find the correlation-exchange energy, but this quantity remains inaccurate. So we have to go beyond DFT to correct this quantity. In this framework, the random phase approximation has gained importance far beyond its initial field of application, condensed matter physics, materials science, and quantum chemistry. RPA is an approach to accurately calculate the electron correlation energy.