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The calculation of the MP2 correlation energy for extended systems can be viewed as a multi-dimensional integral in the thermodynamic limit, and the standard method for evaluating the MP2 energy can be viewed as a trapezoidal quadrature…

Computational Physics · Physics 2023-04-10 Xin Xing , Xiaoxu Li , Lin Lin

We present a real-space method for computing the random phase approximation (RPA) correlation energy within Kohn-Sham density functional theory, leveraging the low-rank nature of the frequency-dependent density response operator. In…

Computational Physics · Physics 2025-04-03 Boqin Zhang , Shikhar Shah , John E. Pask , Edmond Chow , Phanish Suryanarayana

The direct ring coupled-cluster doubles (drCCD)-based random phase approximation (RPA) has provided an attractive framework for the development and application of RPA-related methods. However, a potential unphysical solution issue recently…

Chemical Physics · Physics 2025-08-18 Ruiheng Song , Xiliang Gong , Hong-Zhou Ye

We explore several random phase approximation (RPA) correlation energy variants within the adiabatic-connection fluctuation-dissipation theorem approach. These variants differ in the way the exchange interactions are treated. One of these…

Chemical Physics · Physics 2014-04-08 János G. Angyán , Ru-Fen Liu , Julien Toulouse , Georg Jansen

We assess the performance of a recently proposed renormalized adiabatic local density approximation (rALDA) for \textit{ab initio} calculations of electronic correlation energies in solids and molecules. The method is an extension of the…

Materials Science · Physics 2014-05-30 Thomas Olsen , Kristian S. Thygesen

The relative energies of different phases or polymorphs of molecular solids can be small, less than a kiloJoule/mol. Reliable description of such energy differences requires high quality treatment of electron correlations, typically beyond…

Chemical Physics · Physics 2024-02-19 Khanh Ngoc Pham , Marcin Modrzejewski , Jiří Klimeš

Practical applications of fragment embedding and closely related local correlation methods critically depend on a judicious choice of a low-level theory to define the local embedding subspace and to capture long-range electrostatic and…

Chemical Physics · Physics 2026-05-14 Ruiheng Song , Xiliang Gong , Aamy Bakry , Hong-Zhou Ye

We explore different variants of the random phase approximation (RPA) to the correlation energy derived from closed-shell ring-diagram approximations to coupled cluster doubles theory. We implement these variants in range-separated…

Chemical Physics · Physics 2011-09-01 Julien Toulouse , Wuming Zhu , Andreas Savin , Georg Jansen , János G. Angyán

A fast method is developed for calculating the Random-Phase-Approximation (RPA) correlation energy for density functional theory. The correlation energy is given by a trace over a projected RPA response matrix and the trace is taken by a…

Chemical Physics · Physics 2013-01-01 Daniel Neuhauser , Eran Rabani , Roi Baer

Pair atomic density fitting (PADF) is a promising strategy to reduce the scaling with system size of quantum chemical methods for the calculation of the correlation energy like the direct random phase approximation (RPA) or second-order…

Chemical Physics · Physics 2023-03-14 Edoardo Spadetto , Pier Herman Theodoor Philipsen , Arno Förster , Lucas Visscher

With increasing inter-electronic distance, the screening of the electron-electron interaction by the presence of other electrons becomes the dominant source of electron correlation. This effect is described by the random phase approximation…

Chemical Physics · Physics 2022-09-29 Arno Förster

The random phase approximation (RPA) has emerged as a prominent first-principles method in material science, particularly to study the adsorption and chemisorption of small molecules on surfaces. However, its widespread application is…

Materials Science · Physics 2025-09-01 Edoardo Spadetto , Pier Herman Theodoor Philipsen , Arno Förster , Lucas Visscher

Coupled-cluster theory with single and double excitations (CCSD) is a promising ab initio method for the electronic structure of three-dimensional metals, for which second-order perturbation theory (MP2) diverges in the thermodynamic limit.…

Materials Science · Physics 2021-06-16 James M. Callahan , Malte F. Lange , Timothy C. Berkelbach

The random phase approximation (RPA) systematically overestimates the magnitude of the correlation energy and generally underestimates cohesive energies. This originates in part from the complete lack of exchange terms, which would…

Materials Science · Physics 2018-12-12 Felix Hummel , Andreas Grüneis , Georg Kresse , Paul Ziesche

Analytical forces have been derived in the Lagrangian framework for several random phase approximation (RPA) correlated total energy methods based on the range separated hybrid (RSH) approach, which combines a short-range density functional…

Chemical Physics · Physics 2016-03-16 Bastien Mussard , Peter G. Szalay , János G. Ángyán

Starting from the general expression for the ground state correlation energy in the adiabatic connection fluctuation dissipation theorem (ACFDT) framework, it is shown that the dielectric matrix formulation, which is usually applied to…

Chemical Physics · Physics 2016-04-25 Bastien Mussard , Dario Rocca , Georg Jansen , Janos Angyan

The adiabatic connection fluctuation-dissipation theorem with the random phase approximation (RPA) has recently been applied with success to obtain correlation energies of a variety of chemical and solid state systems. The main merit of…

Materials Science · Physics 2015-03-20 Thomas Olsen , Kristian S. Thygesen

We present an embedding approach to treat local electron correlation effects in periodic environments. In a single, consistent framework, our plane-wave based scheme embeds a local high-level correlation calculation (here Coupled Cluster…

Chemical Physics · Physics 2021-01-07 Tobias Schäfer , Florian Libisch , Georg Kresse , Andreas Grüneis

The accurate computation of non-linear optical properties (NLOPs) in large polymers requires accounting for electronic correlation effects with a reasonable computational cost. The Random Phase Approximation (RPA) used in the adiabatic…

We report an improved implementation for evaluating the analytical gradients of the random phase approximation (RPA) electron-correlation energy based on atomic orbitals and the localized resolution of identity scheme. The more efficient…

Materials Science · Physics 2024-04-17 Muhammad N. Tahir , Honghui Shang , Jia Li , Xinguo Ren
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