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By combining extrapolated selected configuration interaction (sCI) energies obtained with the CIPSI (Configuration Interaction using a Perturbative Selection made Iteratively) algorithm with the recently proposed short-range…

Chemical Physics · Physics 2020-06-05 Emmanuel Giner , Anthony Scemama , Julien Toulouse , Pierre-François Loos

Accurate yet efficient modeling of chemical systems with pronounced static correlation in their excited states remains a significant challenge in quantum chemistry, as most electronic structure methods that can adequately capture static…

Chemical Physics · Physics 2025-03-07 Sylvia J. Bintrim , Kevin Carter-Fenk

We present analytic gradients and derivative couplings for the simplest possible multireference configuration interaction method, CIS-1D, an electronic structure ansatz that includes all single excitations and one lone double excitation on…

Chemical Physics · Physics 2021-02-15 Hung-Hsuan Teh , Joseph E. Subotnik

In this study, we extend the multicomponent heat-bath configuration interaction (HCI) method to excited states. Previous multicomponent HCI studies have been performed using only the variational stage of the HCI algorithm as they have…

Chemical Physics · Physics 2022-01-12 Naresh Alaal , Kurt R. Brorsen

We present a novel randomized block coordinate descent method for the minimization of a convex composite objective function. The method uses (approximate) partial second-order (curvature) information, so that the algorithm performance is…

Optimization and Control · Mathematics 2018-02-28 Kimon Fountoulakis , Rachael Tappenden

Phase retrieval aims at recovering a complex-valued signal from magnitude-only measurements, which attracts much attention since it has numerous applications in many disciplines. However, phase recovery involves solving a system of…

Information Theory · Computer Science 2017-06-13 Wen-Jun Zeng , H. C. So

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

In this work, we revisited the idea of using the coupled-cluster ground state formalism to target excited states. Our main focus was targeting doubly excited states and double core hole states. Typical equation-of-motion (EOM) approaches…

Chemical Physics · Physics 2019-12-04 Joonho Lee , David W. Small , Martin Head-Gordon

We introduce state-averaging into the method of Monte Carlo configuration interaction (SA-MCCI) to allow the stable and efficient calculation of excited states. We show that excited potential curves for H$_{3}$, including a crossing with…

Chemical Physics · Physics 2014-03-03 J. P. Coe , M. J. Paterson

We present a quantum-classical hybrid algorithm for calculating the ground state and its energy of the quantum many-body Hamiltonian by proposing an adaptive construction of a quantum state for the quantum-selected configuration interaction…

Quantum Physics · Physics 2024-12-12 Yuya O. Nakagawa , Masahiko Kamoshita , Wataru Mizukami , Shotaro Sudo , Yu-ya Ohnishi

Striving to define very accurate vertical transition energies, we perform both high-level coupled cluster (CC) calculations (up to CCSDTQP) and selected configuration interaction (sCI) calculations (up to several millions of determinants)…

Downfolding coupled cluster (CC) techniques are powerful tools for reducing the dimensionality of many-body quantum problems. This work investigates how ground-state downfolding formalisms can target excited states using non-Aufbau…

Chemical Physics · Physics 2023-10-24 Nicholas P. Bauman

We investigate configuration-interaction (CI) calculations on a basis of molecular orbitals generated by preliminary density-functional theory (DFT) calculations. We use this CI/DFT framework to improve the modeling of core-excited states…

Chemical Physics · Physics 2025-09-11 Giorgio Visentin , Francois Mauger

We study several approaches to orbital optimization in selected configuration interaction plus perturbation theory (SCI+PT) methods, and test them on the ground and excited states of three molecules using the semistochastic heatbath…

Chemical Physics · Physics 2021-07-14 Yuan Yao , C. J. Umrigar

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

We extend the CIPSI-driven CC($P$;$Q$) methodology [K. Gururangan et al., J. Chem. Phys. 155 (2021) 174114], in which the leading higher-than-doubly excited determinants are identified using the selected configuration interaction (CI)…

Chemical Physics · Physics 2026-02-24 Swati S. Priyadarsini , Karthik Gururangan , Piotr Piecuch

An iterative configuration interaction (iCI)-based multiconfigurational self-consistent field (SCF) theory, iCISCF, is proposed to handle systems that require large complete active spaces (CAS). The success of iCISCF stems from three…

Chemical Physics · Physics 2021-06-21 Yang Guo , Ning Zhang , Yibo Lei , Wenjian Liu

Addressing both dynamic and static correlation accurately is a primary goal in electronic structure theory. Non-orthogonal configuration interaction (NOCI) is a versatile tool for treating static correlation, offering chemical insights by…

Chemical Physics · Physics 2025-06-27 Chong Sun , Fei Gao , Gustavo E. Scuseria

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

We propose an efficient deterministic method to calculate the full configuration interaction (FCI) ground state energy. This method leverages the sparseness of the Lanczos basis vectors that span the Krylov subspace associated with the…

Chemical Physics · Physics 2024-01-08 Lijun Wang