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We report an efficient algorithm using density fitting for the relativistic complete active space self-consistent field (CASSCF) method, which is significantly more stable than the algorithm previously reported by one of the authors [J. E.…

Chemical Physics · Physics 2018-08-01 Ryan D. Reynolds , Takeshi Yanai , Toru Shiozaki

A new iterative solver is proposed to efficiently calculate the ground state electronic structure in Density Functional Theory calculations. This algorithm is particularly useful for simulating physical systems considered difficult to…

Computational Physics · Physics 2021-11-24 Jean-Luc Fattebert

We use the recently-developed Heat-bath Configuration Interaction (HCI) algorithm as an efficient active-space solver to perform multi-configuration self-consistent field calculations (HCISCF) with large active spaces. We give a detailed…

Chemical Physics · Physics 2018-11-08 James E. T. Smith , Adam A. Holmes , Bastien Mussard , Sandeep Sharma

We present a novel implementation of the complete active space self-consistent field (CASSCF) method that makes use of the many-body expanded full configuration interaction (MBE-FCI) method to incrementally approximate electronic structures…

The development of a novel exact two-component (X2C) scheme with the inclusion of the picture-change correction for the fluctuation potential, the X2Ccorr scheme, is reported, hereby establishing a hierarchy of X2C schemes with systematic…

Chemical Physics · Physics 2026-03-02 Xubo Wang , Sen Wang , Yixuan Wu , Lan Cheng

In this paper we provide a detailed convergence analysis for an unconditionally energy stable, second-order accurate convex splitting scheme for the Modified Phase Field Crystal equation, a generalized damped wave equation for which the…

Numerical Analysis · Mathematics 2012-08-08 Arvind Baskaran , John Lowengrub , Cheng Wang , Steve Wise

Although many programs have been published for fully numerical Hartree--Fock (HF) or density functional (DF) calculations on atoms, we are not aware of any that support hybrid DFs, which are popular within the quantum chemistry community…

Chemical Physics · Physics 2019-08-19 Susi Lehtola

We report the derivation and implementation of orbital optimization algorithms for the active space decomposition (ASD) model, which are extensions of complete active space self-consistent field (CASSCF) and its occupation-restricted…

Chemical Physics · Physics 2015-08-17 Inkoo Kim , Shane M. Parker , Toru Shiozaki

We present the One-orbital Ensemble Self-Consistent Field (OE-SCF) method, an {alternative} orbital-free DFT solver that extends the applicability of DFT to system sizes beyond the nanoscale while retaining the accuracy required to be…

Materials Science · Physics 2021-05-05 Xuecheng Shao , Wenhui Mi , Michele Pavanello

We describe an active-set method for the minimization of an objective function $\phi$ that is the sum of a smooth convex function and an $\ell_1$-regularization term. A distinctive feature of the method is the way in which active-set…

Optimization and Control · Mathematics 2015-05-19 Nitish Shirish Keskar , Jorge Nocedal , Figen Oztoprak , Andreas Waechter

In several recent works \cite{Causley2013a}, \cite{Causley2013}, we developed a new second order, A-stable approach to wave propagation problems based on the method of lines transpose (MOL$^T$) formulation combined with alternating…

Numerical Analysis · Mathematics 2013-08-15 Matthew F. Causley , Andrew J. Christlieb

We present a method to perform fully selfconsistent density-functional calculations, which scales linearly with the system size and which is well suited for very large systems. It uses strictly localized pseudoatomic orbitals as basis…

Condensed Matter · Physics 2009-10-28 Pablo Ordejon , Emilio Artacho , Jose M. Soler

In ground-based astronomy, Adaptive Optics (AO) is a pivotal technique, engineered to correct wavefront phase distortions and thereby enhance the quality of the observed images. Integral to an AO system is the wavefront sensor (WFS), which…

Instrumentation and Methods for Astrophysics · Physics 2026-05-07 Yutong Wu , Roland Wagner , Ronny Ramlau , Raymond H. Chan

This work presents a general framework for deriving exact and approximate Newton self-consistent field (SCF) orbital optimization algorithms by leveraging concepts borrowed from differential geometry. Within this framework, we extend the…

Chemical Physics · Physics 2023-09-13 Robin Feldmann , Alberto Baiardi , Markus Reiher

It is shown for two electron atoms that ground-state wavefunctions of the form \begin{equation} \Psi(\vec{r_{1}}, \vec{r_{2}})=\phi(\vec{r_{1}})\phi(\vec{r_{2}})(\cosh ar_{1}+\cosh ar_{2})(1+0.5 r_{12}e^{-b r_{12}}) \end{equation} where…

Atomic Physics · Physics 2015-06-04 Rabeet Singh Chauhan , Manoj K. Harbola

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…

Computational Physics · Physics 2015-12-23 Swarnava Ghosh , Phanish Suryanarayana

We extend the active space decomposition method, recently developed by us, to more than two active sites using the density matrix renormalization group algorithm. The fragment wave functions are described by complete or restricted…

Chemical Physics · Physics 2014-12-09 Shane M. Parker , Toru Shiozaki

The complete active space self-consistent field (CASSCF) method is the principal approach employed for studying strongly correlated systems. However, exact CASSCF can only be performed on small active spaces of ~20 electrons in ~20 orbitals…

Computational Physics · Physics 2021-12-22 Daniel S. Levine , Diptarka Hait , Norm M. Tubman , Susi Lehtola , K. Birgitta Whaley , Martin Head-Gordon

As a follow up to \cite{Causley2013}, we provide a detailed description of the numerical implementation of an O(N), A-stable, second order accurate solution of the wave equation, constructed from semi-discrete boundary value problems. We…

Numerical Analysis · Mathematics 2013-07-01 Matthew F. Causley , Andrew J. Christlieb , Yaman Guclu , Eric Wolf
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