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We have carried out quantum Monte Carlo (QMC) calculations of silicon crystal focusing on the accuracy and systematic biases that affect the electronic structure characteristics. The results show that 64 and 216 atom supercells provide an…

Materials Science · Physics 2021-05-26 Abdulgani Annaberdiyev , Guangming Wang , Cody A. Melton , M. Chandler Bennett , Lubos Mitas

In this work, we introduce a simple modification of the Monte Carlo algorithm, which we call step Monte Carlo (sMC). The sMC approach allows to simulate processes far from equilibrium and obtain information about the dynamic properties of…

Other Condensed Matter · Physics 2023-12-15 Dariusz Sztenkiel

In this communication, we propose a method for obtaining isolated excited states within the Full Configuration Interaction Quantum Monte Carlo framework. This method allows for stable sampling with respect to collapse to lower energy states…

Strongly Correlated Electrons · Physics 2014-10-10 George H. Booth , Garnet Kin-Lic Chan

The electronic structure of the ICl+ molecular ion is investigated by using high-level multireference configuration interaction (MRCI) method. To improve computational accuracy, Davidson corrections, spin-orbit coupling (SOC), and…

Atomic Physics · Physics 2025-11-25 Rui Li , Ronglong Dou , Ting Gao , Qinan Li , Chaoqun Song

We present high-accuracy correlated calculations of small Si$_x$H$_y$ molecular systems both in the ground and excited states. We employ quantum Monte Carlo (QMC) together with a variety of many-body wave function approaches based on basis…

Chemical Physics · Physics 2020-10-21 Guangming Wang , Abdulgani Annaberdiyev , Lubos Mitas

State-specific electronic structure theory provides a route towards balanced excited-state wave functions by exploiting higher-energy stationary points of the electronic energy. Multiconfigurational wave function approximations can describe…

Chemical Physics · Physics 2023-07-19 Antoine Marie , Hugh G. A. Burton

We introduce natural transition geminals as a means to qualitatively understand a transition where double excitations are important. The first two $A_{1}$ singlet states of the CH cation are used as an initial example. We calculate these…

Chemical Physics · Physics 2014-03-11 J. P. Coe , M. J. Paterson

While configuration interaction singles (CIS) provides a computationally efficient description of excited states, it systematically overestimates excitation energies and performs poorly for strongly correlated systems, partly due to the…

Chemical Physics · Physics 2026-04-01 Takashi Tsuchimochi , Benjamin Mokhtar

Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017); J. Chem. Phys. 154, 124103 (2021)], we propose a novel…

Chemical Physics · Physics 2022-10-06 Karthik Gururangan , J. Emiliano Deustua , Jun Shen , Piotr Piecuch

We introduce and benchmark a systematically improvable route for excited-state calculations, state-specific configuration interaction ($\Delta$CI), \alert{which is a particular realization of multiconfigurational self-consistent field and…

Chemical Physics · Physics 2023-08-31 Fábris Kossoski , Pierre-François Loos

Accurate determination of electronic properties of correlated oxides remains a significant challenge for computational theory. Traditional Hubbard-corrected density functional theory (DFT+U) frequently encounters limitations in precisely…

Materials Science · Physics 2024-03-19 Hyeondeok Shin , Kevin Gasperich , Tomas Rojas , Anh T. Ngo , Jaron T. Krogel , Anouar Benali

We introduce the multistate iterative qubit coupled cluster (MS-iQCC) method, a quantum-inspired algorithm that runs efficiently on classical hardware and is designed to predict both ground and excited electronic states of molecules.…

Chemical Physics · Physics 2026-01-05 Robert A. Lang , Shashank G. Mehendale , Ilya G. Ryabinkin , Artur F. Izmaylov

The concept of machine learning configuration interaction (MLCI) [J. Chem. Theory Comput. 2018, 14, 5739], where an artificial neural network (ANN) learns on the fly to select important configurations, is further developed so that accurate…

Chemical Physics · Physics 2019-10-31 J. P. Coe

We describe and discuss a recently proposed quantum Monte Carlo algorithm to compute the ground-state properties of various systems of interacting fermions. In this method, the ground state is projected from an initial wave function by a…

Condensed Matter · Physics 2009-10-28 Shiwei Zhang , J. Carlson , J. E. Gubernatis

The recently proposed many-body expanded full configuration interaction (MBE-FCI) method is extended to excited states and static first-order properties different from total, ground state correlation energies. Results are presented for…

Chemical Physics · Physics 2020-10-20 Janus J. Eriksen , Jürgen Gauss

We calculate accurate potential energy curves for a ground-state He$^+$ ion interacting with a He atom in the lowest-energy metastable $^3\!S$ electronic state. We employ the full configuration interaction method, equivalent to exact…

Atomic Physics · Physics 2023-11-30 Jacek Gȩbala , Michał Przybytek , Marcin Gronowski , Michał Tomza

We extend our hybrid linear-method/accelerated-descent variational Monte Carlo optimization approach to excited states and investigate its efficacy in double excitations. In addition to showing a superior statistical efficiency when…

Chemical Physics · Physics 2022-02-24 Leon Otis , Isaac M. Craig , Eric Neuscamman

The mean-field solutions of electronic excited states are much less accessible than ground state (e.g.\ Hartree-Fock) solutions. Energy-based optimization methods for excited states, like $\Delta$-scf, tend to fall into the lowest solution…

Chemical Physics · Physics 2022-10-11 Hong-Zhou Ye , Matthew Wellborn , Nathan D. Ricke , Troy Van Voorhis

Neural-network wave functions in Variational Monte Carlo (VMC) have achieved great success in accurately representing both ground and excited states. However, achieving sufficient numerical accuracy in state overlaps requires increasing the…

Machine Learning · Computer Science 2026-05-28 Nicholas Gao , Till Grutschus , Frank Noé , Stephan Günnemann

Accurate ab initio calculations of 3d transition metal monoxide molecules have attracted extensive attention because of its relevance in physical and chemical science, as well as theoretical challenges in treating strong electron…

Strongly Correlated Electrons · Physics 2021-11-02 Tonghuan Jiang , Yilin Chen , Nikolay Bogdanov , Enge Wang , Ali Alavi , Ji Chen