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Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body…

Chemical Physics · Physics 2019-12-12 Janus J. Eriksen , Jürgen Gauss

In a recent paper, we proposed the adaptive shift method for correcting the undersampling bias of the initiator-FCIQMC. The method allows faster convergence with the number of walkers to the FCI limit than the normal initiator method,…

Computational Physics · Physics 2021-02-03 Khaldoon Ghanem , Kai Guther , Ali Alavi

The choice of molecular orbitals is decisive in configuration interaction calculations. In this letter, a democratic description of the ground and excited states follows an orthogonally constrained orbitals optimization to produce…

Quantum Physics · Physics 2023-02-16 Saad Yalouz , Vincent Robert

Over the course of the past few decades, the field of computational chemistry has managed to manifest itself as a key complement to more traditional lab-oriented chemistry. This is particularly true in the wake of the recent renaissance of…

Chemical Physics · Physics 2018-10-16 Janus J. Eriksen , Jürgen Gauss

Non-orthogonal configuration interaction (NOCI) is a generalization of the standard orthogonal configuration interaction (CI) method and offers a highly flexible framework for describing ground and excited electronic states. However, this…

Chemical Physics · Physics 2024-12-24 Daniel Graf , Alex J. W. Thom

We present a fully variational locally scaled self-interaction corrected (SIC) energy functional using complex optimal orbitals. This represents an important milestone for fully variational SIC energy functionals, which have been shown to…

We present an efficient orbital optimization procedure that combines the highly GPU accelerated, spin-adapted density matrix renormalization group (DMRG) method with the complete active space self-consistent field (CAS-SCF) approach for…

In a previous paper we proposed a Projected Configuration Interaction method that uses sets of axially deformed single particle states to build up the many body basis. We show that the choice of the basis set is essential for the efficiency…

Nuclear Theory · Physics 2013-05-29 Zao-Chun Gao , Mihai Horoi , Y. S. Chen

The Configuration Interaction (CI) method using orbitals centered on the nucleus has recently been applied to calculate the interactions of positrons interacting with atoms. Computational investigations of the convergence properties of…

Atomic Physics · Physics 2007-05-23 J. Mitroy , M. W. J. Bromley

This work explores the ability of classical electronic structure methods to efficiently represent (compress) the information content of full configuration interaction (FCI) wave functions. We introduce a benchmark set of four hydrogen model…

Chemical Physics · Physics 2020-08-20 Nicholas H. Stair , Francesco A. Evangelista

According to the modern paradigms of software engineering, standard tasks are best accomplished by reusable open source libraries. We describe OpenOrbitalOptimizer: a reusable open source C++ library for the iterative solution of coupled…

Computational Physics · Physics 2025-06-03 Susi Lehtola , Lori A. Burns

A stochastic configuration interaction method based on evolutionary algorithm is designed as an affordable approximation to full configuration interaction (FCI). The algorithm comprises of initiation, propagation and termination steps,…

Strongly Correlated Electrons · Physics 2016-08-18 Rahul Chakraborty , Debashree Ghosh

Configuration Interaction (CI) calculations on the ground state of the C atom are carried out using a small basis set of Slater orbitals [7s6p5d4f3g]. The configurations are selected according to their contribution to the total energy. One…

Atomic Physics · Physics 2017-08-01 María Belén Ruiz , Robert Tröger

A new large-scale parallel multiconfigurational self-consistent field (MCSCF) implementation in the open-source NWChem computational chemistry code is presented. The generalized active space (GAS) approach is used to partition large…

Chemical Physics · Physics 2026-01-06 Konstantinos D. Vogiatzis , Dongxia Ma , Jeppe Olsen , Laura Gagliardi , Wibe de Jong

The recent many-body expanded full configuration interaction (MBE-FCI) method is reviewed by critically assessing its advantages and drawbacks in the context of contemporary near-exact electronic structure theory. Besides providing a…

Chemical Physics · Physics 2021-03-02 Janus J. Eriksen , Jürgen Gauss

Fermi-L\"owdin orbital self-interaction-correction (FLOSIC) method uses symmetric orthogonalized Fermi orbitals as localized orbitals in one-electron SIC schemes. In FLOSIC, a set of Fermi orbital descriptors (FOD) that define the FLOs is…

Chemical Physics · Physics 2025-08-08 Selim Romero , Yoh Yamamoto , Tunna Baruah , Rajendra R. Zope

Interpretations of logical formulas over semirings have applications in various areas of computer science including logic, AI, databases, and security. Such interpretations provide richer information beyond the truth or falsity of a…

Logic in Computer Science · Computer Science 2023-02-28 A. Pavan , Kuldeep S. Meel , N. V. Vinodchandran , Arnab Bhattacharyya

We present three modifications to our recently introduced fast randomized iteration method for full configuration interaction (FCI-FRI) and investigate their effects on the method's performance for Ne, H$_2$O, and N$_2$. The initiator…

Computational Physics · Physics 2023-10-03 Samuel M. Greene , Robert J. Webber , Jonathan Weare , Timothy C. Berkelbach

Ab initio calculations face the challenge of describing a complex multiscale quantum many-body system. The nuclear wave function has both strong short-range correlations and long-range contributions. Natural orbitals provide a means of…

Nuclear Theory · Physics 2017-04-11 Chrysovalantis Constantinou

We present an approach to combining selected configuration interaction (SCI) and initiator full configuration interaction quantum Monte Carlo (i-FCIQMC). In the current i-FCIQMC scheme, the space of initiators is chosen dynamically by a…

Chemical Physics · Physics 2019-11-15 Nick S. Blunt