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The time-dependent restricted-active-space self-consistent-field singles (TD-RASSCF-S) method is presented for investigating TD many-electron dynamics in atoms and molecules. Adopting the SCF notion from the muticonfigurational TD…

Atomic Physics · Physics 2014-05-22 Haruhide Miyagi , Lars Bojer Madsen

Complete active space self-consistent field (CASSCF) computations can be realized at polynomial cost via the variational optimization of the active-space two-electron reduced-density matrix (2-RDM). Like conventional approaches to CASSCF,…

Chemical Physics · Physics 2018-12-10 Mohammad Mostafanejad , A. Eugene DePrince

We present a numerical implementation of the infinite-range exterior complex scaling (irECS) [Phys. Rev. A 81, 053845 (2010)] as an efficient absorbing boundary to the time-dependent complete-active-space self-consistent field (TD-CASSCF)…

Atomic Physics · Physics 2018-03-07 Yuki Orimo , Takeshi Sato , Armin Scrinzi , Kenichi L. Ishikawa

We present a fully variational generalization of the pseudo self-interaction correction (VPSIC) approach previously presented in two implementations based on plane-waves and atomic orbital basis set, known as PSIC and ASIC, respectively.…

Materials Science · Physics 2015-05-28 A. Filippetti , C. D. Pemmaraju , P. Delugas , D. Puggioni , V. Fiorentini , S. Sanvito

The multi-configurational self-consistent field theory is considered the standard starting point for almost all multireference approaches required for strongly-correlated molecular problems. The limitation of the approach is generally given…

Chemical Physics · Physics 2015-10-14 Robert E. Thomas , Qiming Sun , Ali Alavi , George H. Booth

We have combined our adaptive configuration interaction (ACI) [J.B. Schriber and F.A. Evangelista, J. Chem. Phys. 144, 161106 (2016)] with a density-fitted implementation of the second-order perturbative multireference driven similarity…

Chemical Physics · Physics 2018-08-29 Jeffrey B. Schriber , Kevin P. Hannon , Francesco A. Evangelista

The most essential concept in concurrent multiscale methods involving atomistic-continuum coupling is how to define the relation between atomistic and continuum regions. A well-known coupling method that has been frequently employed in…

Mesoscale and Nanoscale Physics · Physics 2022-07-27 Pouya Towhidi , Manouchehr Salehi

Adiabatic connection models (ACMs), which interpolate between the limits of weak and strong interaction, are powerful tools to build accurate exchange-correlation functionals. If the exact weak-interaction expansion from second-order…

Chemical Physics · Physics 2022-09-08 S. Śmiga , F. Della Sala , P. Gori-Giorgi , E. Fabiano

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

For many-body methods such as MCSCF and CASSCF, in which the number of one-electron orbitals are optimized and independent of basis set used, there are no problems with using plane-wave basis sets. However, for methods currently used in…

Computational Physics · Physics 2020-09-02 Eric J. Bylaska , Duo Song , Nicholas P. Bauman , Karol Kowalski , Daniel Claudino , Travis S. Humble

An externally corrected coupled cluster (CC) method, where an adaptive configuration interaction (ACI) wave function provides the external cluster amplitudes, named ACI-CC, is presented. By exploiting the connection between configuration…

Chemical Physics · Physics 2023-09-27 Gustavo J. R. Aroeira , Madeline M. Davis , Justin M. Turney , Henry F. Schaefer

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

Although selected configuration interaction (SCI) algorithms can tackle much larger Hilbert spaces than the conventional full CI (FCI) method, the scaling of their computational cost with respect to the system size remains inherently…

Chemical Physics · Physics 2024-12-02 Abdallah Ammar , Anthony Scemama , Pierre-François Loos , Emmanuel Giner

We report the derivation and implementation of orbital optimization algorithms for the active space decomposition (ASD) model, which are extensions of complete active space self-consistent field (CASSCF) and its occupation-restricted…

Chemical Physics · Physics 2015-08-17 Inkoo Kim , Shane M. Parker , Toru Shiozaki

The development of variational density functional theory approaches to excited electronic states is impeded by limitations of the commonly used self-consistent field (SCF) procedure. A method based on a direct optimization approach as well…

Chemical Physics · Physics 2022-11-09 Gianluca Levi , Aleksei V. Ivanov , Hannes Jónsson

The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…

Chemical Physics · Physics 2024-05-03 Yannick J. Franzke , Werner M. Schosser , Fabian Pauly

Recently proposed local self-interaction correction (LSIC) method [Zope, R. R. et al., J. Chem. Phys. 151, 214108 (2019)] is a one-electron self-interaction-correction (SIC) method that uses an iso-orbital indicator to apply the SIC at each…

Chemical Physics · Physics 2023-02-22 Yoh Yamamoto , Tunna Baruah , Po-Hao Chang , Selim Romero , Rajendra R. Zope

Quantum Selected Configuration Interaction (QSCI) methods (also known as Sample-based Quantum Diagonalization, SQD) have emerged as promising near-term approaches to solving the electronic Schr{\"o}dinger equation with quantum computers. In…

We derive and implement analytic nuclear gradients and derivative couplings for a constrained Complete Active Space Self-Consistent Field with a small active space designed to model electron or hole transfer. Using a Lagrangian formalism,…

Computational Physics · Physics 2025-09-01 Tian Qiu , Joseph E. Subotnik

Single-molecule magnets (SMMs) are promising candidates for molecular-scale data storage and processing due to their strong magnetic anisotropy and long spin relaxation times. However, as temperature rises, interactions between electronic…

Materials Science · Physics 2024-12-11 Soumi Haldar , Lorenzo A. Mariano , Alessandro Lunghi , Laura Gagliardi