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We introduce a new procedure for iterative selection of determinant spaces capable of describing highly correlated systems. This adaptive configuration interaction (ACI) determines an optimal basis by an iterative procedure in which the…

Chemical Physics · Physics 2016-05-25 Jeffrey B. Schriber , Francesco A. Evangelista

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

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

We present quantum algorithms, for Hamiltonians of linear combinations of local unitary operators, for Hamiltonian matrix-vector products and for preconditioning with the inverse of shifted reduced Hamiltonian operator that contributes to…

Quantum Physics · Physics 2020-09-09 Zhiyong Zhang

Asymptotics-based configuration-interaction (CI) methods [G. Friesecke and B. D. Goddard, Multiscale Model. Simul. 7, 1876 (2009)] are a class of CI methods for atoms which reproduce, at fixed finite subspace dimension, the exact…

Quantum Physics · Physics 2012-04-06 Christian Mendl , Gero Friesecke

In this work, we extend selected configuration interaction (SCI) methods beyond energies and expectation values by introducing a linear response (LR) framework for molecular response properties. Existing SCI approaches are capable of…

Chemical Physics · Physics 2025-11-24 Peter Reinholdt , Erik Kjellgren , Jacob Kongsted

A recent direction in quantum computing for molecular electronic structure sees the use of quantum devices as configuration sampling machines integrated within high-performance computing (HPC) platforms. This appeals to the strengths of…

Quantum Physics · Physics 2026-05-18 Tim Weaving , Angus Mingare , Alexis Ralli , Peter V. Coveney

In a recent work, we introduced the foundations of an orthogonally constrained complete active space self-consistent field (OC-CASSCF) framework that produces state-specific molecular orbitals for mutually orthogonal multiconfigurational…

Chemical Physics · Physics 2026-01-28 Loris Delafosse , Vincent Robert , Saad Yalouz

High-precision atomic structure calculations require accurate modelling of electronic correlations typically addressed via the configuration interaction (CI) problem on a multiconfiguration wave function expansion. The latter can easily…

Atomic Physics · Physics 2023-06-22 Pavlo Bilous , Adriana Pálffy , Florian Marquardt

We present a self consistent field approach (SCF) within the Adaptive Derivative-Assembled Problem-Tailored Ansatz Variational Quantum Eigensolver (ADAPT-VQE) framework for efficient quantum simulations of chemical systems on near-term…

We propose using the wave function generated by the quantum selected configuration interaction (QSCI) method as the trial wave function in phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC). In the QSCI framework, electronic…

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

Many-body simulations of quantum systems is an active field of research that involves many different methods targeting various computing platforms. Many methods commonly employed, particularly coupled cluster methods, have been adapted to…

Chemical Physics · Physics 2023-06-14 David B. Williams-Young , Norm M. Tubman , Carlos Mejuto-Zaera , Wibe A. de Jong

By combining Hartree-Fock with a neural-network-supported quantum-cluster solver proposed recently in the context of solid-state lattice models, we formulate a scheme for selective neural-network configuration interaction (NNCI)…

Quantum-selected configuration interaction (QSCI) is an approach for quantum chemical calculations using current quantum computers. In conventional QSCI, Slater determinants used for the wave function expansion are sampled by iteratively…

Quantum Physics · Physics 2025-10-03 Kenji Sugisaki , Shu Kanno , Toshinari Itoko , Rei Sakuma , Naoki Yamamoto

It has recently been shown that the SOiCI approach [J. Phys.: Condens. Matter 34 (2022) 224007], in conjunction with the spin-separated exact two-component relativistic Hamiltonian, can provide very accurate fine structures of systems…

Chemical Physics · Physics 2023-07-18 Yang Guo , Ning Zhang , Wenjian Liu

We develop an efficient algorithm, coordinate descent FCI (CDFCI), for the electronic structure ground state calculation in the configuration interaction framework. CDFCI solves an unconstrained non-convex optimization problem, which is a…

Chemical Physics · Physics 2019-07-03 Zhe Wang , Yingzhou Li , Jianfeng Lu

The combinatorial scaling of configuration interaction (CI) has long restricted its applicability to only the simplest molecular systems. Here, we report the first numerically exact CI calculation exceeding one quadrillion ($10^{15}$)…

Chemical Physics · Physics 2025-12-16 Agam Shayit , Can Liao , Shiv Upadhyay , Hang Hu , Tianyuan Zhang , Eugene DePrince , Chao Yang , Xiaosong Li

In a previous work (arXiv:2010.02027) we showed how the full configuration interaction (FCI) ground state energy can be obtained as a functional of an arbitrary reference wavefunction by means of a gradient descent or quasi-Newton…

Chemical Physics · Physics 2020-12-10 Carlos A. Jiménez-Hoyos

Full configuration interaction (FCI) solvers are limited to small basis sets due to their expensive computational costs. An optimal orbital selection for FCI (OptOrbFCI) is proposed to boost the power of existing FCI solvers to pursue the…

Chemical Physics · Physics 2020-09-01 Yingzhou Li , Jianfeng Lu