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We describe our efforts of the past few years to create a large set of more than 500 highly-accurate vertical excitation energies of various natures ($\pi \to \pi^*$, $n \to \pi^*$, double excitation, Rydberg, singlet, doublet, triplet,…

We introduce a hybrid many-body approach that combines the flexibility of the No-Core Shell Model (NCSM) with the efficiency of Multi-Configurational Perturbation Theory (MCPT) to compute ground- and excited-state energies in arbitrary…

Nuclear Theory · Physics 2018-10-24 Alexander Tichai , Eskendr Gebrerufael , Klaus Vobig , Robert Roth

Quantum computing methods for excited-state calculations remain underexplored in Noisy Intermediate-Scale Quantum (NISQ) hardware, despite their critical role in photochemistry and material science. Herein, we propose a resource-efficient…

Quantum Physics · Physics 2025-06-16 Qianjun Yao , He Li

We report an efficient implementation of a second-order multireference perturbation theory based on the driven similarity renormalization group (DSRG-MRPT2) [C. Li and F. A. Evangelista, J. Chem. Theory Comput. 11, 2097 (2015)]. Our…

Chemical Physics · Physics 2016-06-22 Kevin P. Hannon , Chenyang Li , Francesco A. Evangelista

In this work we propose a chemically-informed data-driven approach to benchmark the approximate density-functional tight-binding (DFTB) excited state (ES) methods that are currently available within the DFTB+ suite. By taking advantage of…

Chemical Physics · Physics 2023-01-02 Andrés I. Bertoni , Cristián G. Sánchez

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

In single-reference coupled-cluster (CC) methods, one has to solve a set of non-linear polynomial equations in order to determine the so-called amplitudes which are then used to compute the energy and other properties. Although it is of…

Chemical Physics · Physics 2021-09-10 Antoine Marie , Fábris Kossoski , Pierre-François Loos

We present a method for calculation of the second-order exchange-dispersion energy in the framework of the symmetry-adapted perturbation theory (SAPT) for weakly interacting monomers described with multiconfigurational wave functions. The…

Chemical Physics · Physics 2019-10-11 Hapka Michał , Przybytek Michał , Pernal Katarzyna

In spite of missing dynamical correlations, the projected generator coordinate method (PGCM) was recently shown to be a suitable method to tackle the low-lying spectroscopy of complex nuclei. Still, describing absolute binding energies and…

Perturbative and non-perturbative expansion methods already constitute a tool of choice to perform ab initio calculations over a significant part of the nuclear chart. In this context, the categories of accessible nuclei directly reflect…

Nuclear Theory · Physics 2022-01-28 Mikael Frosini , Thomas Duguet , Jean-Paul Ebran , Vittorio Somà

Full Configuration Interaction Quantum Monte Carlo (FCIQMC) has been effectively applied to very large configuration interaction (CI) problems, and was recently adapted for use as an active space solver and combined with orbital…

Chemical Physics · Physics 2020-02-19 Robert J. Anderson , Toru Shiozaki , George H. Booth

We report theoretical best estimates of vertical transition energies (VTEs) for a large number of excited states and molecules: the \textsc{quest} database. This database includes 1489 \emph{aug}-cc-pVTZ VTEs (731 singlets, 233 doublets,…

The simulation of molecular electronic structure is an important application of quantum devices. Recently, it has been shown that quantum devices can be effectively combined with classical supercomputing centers in the context of the…

Quantum Physics · Physics 2025-02-28 Stefano Barison , Javier Robledo Moreno , Mario Motta

The efficiency of the recently proposed iCIPT2 [iterative configuration interaction (iCI) with selection and second-order perturbation theory (PT2); J. Chem. Theory Comput. 16, 2296 (2020)] for strongly correlated electrons is further…

Chemical Physics · Physics 2020-11-19 Ning Zhang , Wenjian Liu , Mark R. Hoffmann

A third-order multireference perturbation theory based on the driven similarity renormalization group approach (DSRG-MRPT3) is presented. The DSRG-MRPT3 method has several appealing features: a) it is intruder free, b) it is size…

Chemical Physics · Physics 2017-04-26 Chenyang Li , Francesco A. Evangelista

We extend the recently proposed heat-bath configuration interaction (HCI) method [Holmes, Tubman, Umrigar, J. Chem. Theory Comput. 12, 3674 (2016)], by introducing a semistochastic algorithm for performing multireference Epstein-Nesbet…

Chemical Physics · Physics 2017-03-20 Sandeep Sharma , Adam Holmes , Guillaume Jeanmairet , Ali Alavi , C. J. Umrigar

The nuclear-electronic orbital (NEO) approach incorporates nuclear quantum effects into quantum chemistry calculations by treating specified nuclei quantum mechanically, equivalently to the electrons. Within the NEO framework, excited…

Chemical Physics · Physics 2025-03-19 Christopher L. Malbon , Sharon Hammes-Schiffer

In this second part of our series on the recently proposed many-body expanded full configuration interaction (MBE-FCI) method, we introduce the concept of multideterminantal expansion references. Through theoretical arguments and numerical…

Chemical Physics · Physics 2019-09-23 Janus J. Eriksen , Jürgen Gauss

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

The perturbatively selected configuration interaction scheme (CIPSI) is particularly effective in constructing determinantal expansions for quantum Monte Carlo (QMC) simulations with Jastrow-Slater wave functions: fast and smooth…

Classical Physics · Physics 2021-03-02 Monika Dash , Saverio Moroni , Claudia Filippi , Anthony Scemama