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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

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

The computationally expensive evaluation and storage of high-rank reduced density matrices (RDMs) has been the bottleneck in the calculation of dynamic correlation for multireference wave functions in large active spaces. We present a…

Chemical Physics · Physics 2020-01-08 Ankit Mahajan , Nick S. Blunt , Iliya Sabzevari , Sandeep Sharma

We present a natural orbital-based implementation of the intermediate Hamiltonian Fock space coupled-cluster method for (1,1) sector of Fock space. The use of natural orbital significantly reduces the computational cost and can…

Chemical Physics · Physics 2021-09-07 Soumi Haldar , Achintya Kumar Dutta

We develop a stochastic formulation of the optimally-tuned range-separated hybrid density functional theory which enables significant reduction of the computational effort and scaling of the non-local exchange operator at the price of…

Chemical Physics · Physics 2016-09-28 Daniel Neuhauser , Eran Rabani , Yael Cytter , Roi Baer

We present an implementation and analysis of a stochastic high performance algorithm to calculate the correlation energy of three dimensional periodic systems in second-order M{\o}ller-Plesset perturbation theory (MP2). In particular we…

Chemical Physics · Physics 2018-02-12 Tobias Schäfer , Benjamin Ramberger , Georg Kresse

Hybrid multiscale modelling has emerged as a useful framework for modelling complex biological phenomena. However, when accounting for stochasticity in the internal dynamics of agents, these models frequently become computationally…

Quantitative Methods · Quantitative Biology 2021-05-11 Daria Stepanova , Helen M. Byrne , Philip K. Maini , Tomás Alarcón

This work presents a novel approach to distribute orbitals into subspaces within electron-pairing-based natural orbital functionals (NOFs). This approach modifies the coupling between weakly and strongly occupied orbitals by applying an…

Chemical Physics · Physics 2025-02-05 Élodie Boutou , Juan Felipe Huan Lew-Yee , Jose Maria Mercero , Mario Piris

In this paper, we extend the idea of using controlled perturbations to enhance the capabilities of active-set prediction for interior point methods for convex Quadratic Programming (QP) problems. Namely, we consider perturbing the…

Optimization and Control · Mathematics 2014-09-23 Yiming Yan

In earlier work [J. Chem. Phys. 144, 064102 (2016)], we introduced a time-dependent formulation of the second-order N-electron valence perturbation theory (t-NEVPT2) which (i) had a lower computational scaling than the usual…

Chemical Physics · Physics 2018-04-09 Alexander Sokolov , Sheng Guo , Enrico Ronca , Garnet Kin-Lic Chan

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

We present an efficient orbital optimization procedure that combines the highly GPU accelerated, spin-adapted density matrix renormalization group (DMRG) method with the complete active space self-consistent field (CAS-SCF) approach for…

UGA-SSMRPT2, the spin-free perturbative analogue of Mukerjee's State-Specific Multireference Coupled Cluster Theory (MkMRCC) is known to be successful for size-extensive and intruder-free construction of dissociation curves. This work…

Chemical Physics · Physics 2026-02-05 Shamik Chanda , Pratyush Bhattacharjya , Avijit Sen , Sangita Sen

Correlated electron materials, such as superconductors and magnetic materials, are regarded as fascinating targets in quantum computing. However, the quantitative resources, specifically the number of quantum gates and qubits, required to…

Quantum Physics · Physics 2022-08-02 Shu Kanno , Suguru Endo , Takeru Utsumi , Tomofumi Tada

A hybrid stochastic-deterministic approach for computing the second-order perturbative contribution $E^{(2)}$ within multireference perturbation theory (MRPT) is presented. The idea at the heart of our hybrid scheme --- based on a…

Chemical Physics · Physics 2018-05-31 Yann Garniron , Anthony Scemama , Pierre-François Loos , Michel Caffarel

An efficient perturbational treatment of spin-orbit coupling within the framework of high-level multi-reference techniques has been implemented in the most recent version of the COLUMBUS quantum chemistry package, extending the existing…

We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

Intramolecular symmetry-adapted perturbation theory (ISAPT) is a method to compute and decompose the noncovalent interaction energy between two molecular fragments A and B connected via a linker C. The existing ISAPT algorithm displays…

Chemical Physics · Physics 2022-09-13 Du Luu , Konrad Patkowski

Incremental full configuration interaction (iFCI) closely approximates the FCI limit with polynomial cost through a many-body expansion of the correlation energy, providing highly accurate total energies within a given basis set. To extend…

Chemical Physics · Physics 2025-02-26 Jeffrey Hatch , Paul M. Zimmerman

We combine theoretical and experimental efforts to propose a method for studying energy fluctuations, in particular, to obtain the related bi-stochastic matrix of transition probabilities by means of simple measurements at the end of a…

Quantum Physics · Physics 2021-07-21 Marcela Herrera , John P. S. Peterson , Roberto M. Serra , Irene D'Amico