Article
Chemistry, Multidisciplinary
Zsolt Benedek, Paula Timar, Tibor Szilvasi, Gergely Barcza
Summary: In this study, the relation between HF-CC and KS-CC methods is examined by comparing truncated CC calculations to the full configuration interaction. The results show that changing from HF to a KS reference does not lead to systematic improvement in coupled cluster electronic energies, densities, and chemical reaction energies. However, fortuitous error cancellations might occasionally result in illusory improvement compared to HF-CC. Overall, the choice of reference has negligible influence on the results at sufficiently high CC levels, making KS-CC a useful alternative in cases of difficulties with HF or HF-CC convergence.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2022)
Article
Mathematics, Applied
Mihaly A. Csirik, Andre Laestadius
Summary: In this series of articles, we present a comprehensive mathematical framework for Coupled-Cluster-type methods. In the second part, we employ topological degree theory to analyze the nonlinear equations of the single-reference Coupled-Cluster method, obtaining existence results and qualitative information about the solutions. We also calculate the topological index of the zeros of the single-reference Coupled-Cluster mapping and derive an energy error bound for approximate eigenstates of the Schrodinger equation in the truncated Coupled-Cluster method.
ESAIM-MATHEMATICAL MODELLING AND NUMERICAL ANALYSIS
(2023)
Article
Chemistry, Physical
Guillaume Thiam, Franck Rabilloud
Summary: Weakly bound non-valence anions are molecular systems where the excess electron stabilizes in a diffuse orbital governed by the long-range electrostatic potential. DFT-based calculations can describe these systems if a correct asymptotic exchange and correlation potential is used. This provides an alternative to computationally demanding highly correlated method calculations and suggests potential use in constructing new DFT potentials for studying systems with significant nonlocal effects.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Inorganic & Nuclear
Maria Drosou, Christiana A. Mitsopoulou, Dimitrios A. Pantazis
Summary: A detailed study of spin-state energetics for eight Mn(III) and Mn(II) SCO complexes was conducted using a coupled cluster theory approach, leading to the proposal of a robust and efficient computational protocol for studying spin crossover systems. The results highlighted the limitations of multireference wavefunction-based and DFT approaches in providing a balanced description of spin-state energetics for these complexes, underscoring the proposed DLPNO-CCSD(T) protocol as a generally applicable reference-quality quantum chemical method.
Article
Chemistry, Multidisciplinary
Hector H. Corzo, Andreas Erbs Hillers-Bendtsen, Ashleigh Barnes, Abdulrahman Y. Zamani, Filip Pawlowski, Jeppe Olsen, Poul Jorgensen, Kurt V. Mikkelsen, Dmytro Bykov
Summary: This study addresses the computational challenges of investigating complex chemical systems using ab-initio methodologies. The researchers introduce the Divide-Expand-Consolidate (DEC) approach, which is a linear-scaling, massively parallel framework, as a viable solution for coupled cluster (CC) theory. They also present the cluster perturbation theory to mitigate the inherent limitations of DEC. Furthermore, they propose the CPS (D-3) model, derived from a CC singles parent and a doubles auxiliary excitation space, for efficient computation of excitation energies in large molecular systems. Overall, this study provides new algorithms and frameworks that can significantly improve the calculation of molecular properties.
FRONTIERS IN CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Junzi Liu, Lan Cheng
Summary: The article reviews the development of relativistic coupled-cluster and equation-of-motion coupled-cluster methods, focusing on recent efforts to improve computational efficiency and extend the methods to molecules containing heavy elements. Future directions for the development of these methods are also discussed.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2021)
Article
Chemistry, Physical
Ruhee D'Cunha, T. Daniel Crawford
Summary: In this study, the efficacy of two variations of the pair-natural-orbital approach, namely PNO++ and combined PNO++, were investigated for reducing the scaling in coupled cluster property calculations. The results showed that for different types of molecules, the truncation errors in response properties were similar for all three methods, while the PNO method performed slightly better than the PNO++ and combined PNO++ methods in terms of correlation energies.
Article
Chemistry, Physical
Artur Nowak, Ors Legeza, Katharina Boguslawski
Summary: Wave functions based on electron-pair states provide reliable models for describing quantum many-body problems with strongly correlated electrons, especially when broken-pair states are corrected appropriately. The study analyzes the performance of electron-pair methods in predicting orbital-based correlation spectra, focusing on the pCCD-LCC ansatz. It is found that pCCD-LCC accurately reproduces orbital-pair correlation patterns in weak correlation limits and for molecules close to their equilibrium structure.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Erik Rosendahl Kjellgren, Hans Jorgen Aagaard Jensen
Summary: The multi-configurational short-range (sr) density functional theory has been extended to calculate indirect spin-spin coupling constants (SSCCs) for nuclear magnetic resonance spectroscopy. The performance of the new method is compared to other density functional theories, showing that computationally cost-effective srLDA functionals are preferable. In organic compounds, HF-srDFT is the best choice for calculating SSCCs, while CAS-srDFT is needed for fluorine-metals SSCCs.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Review
Chemistry, Multidisciplinary
Benedicte Sverdrup Ofstad, Einar Aurbakken, Oyvind Sigmundson Schoyen, Hakon Emil Kristiansen, Simen Kvaal, Thomas Bondo Pedersen
Summary: In recent years, there has been growing interest in time-dependent coupled-cluster (TDCC) theory for simulating laser-driven electronic dynamics in atoms and molecules, as well as molecular vibrational dynamics. This review covers different types of single-reference TDCC theory based on orthonormal static, orthonormal time-dependent, or biorthonormal time-dependent spin orbitals. The time-dependent extension of equation-of-motion coupled-cluster theory and various applications of TDCC methods are also discussed, including the calculation of linear absorption spectra, response functions, high harmonic generation spectra, and ionization dynamics. Additionally, the role of TDCC theory in finite-temperature many-body quantum mechanics and other application areas is briefly described.
WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
(2023)
Article
Chemistry, Physical
Rahul Chakraborty, Katharina Boguslawski, Pawel Tecmer
Summary: This research proposes a novel wave function theory in a density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster doubles (pCCD)-type methods. The method can reliably describe strongly-correlated systems with mean-field-like computational cost and has been tested for the excitation energies of various molecular structures. The results show that it is an effective computational method for excited states in large molecular systems.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Astronomy & Astrophysics
Cecilia Nagy, Zoltan Keresztes, Laszlo A. Gergely
Summary: The study explores black hole solutions of Horndeski scalar-tensor theory using a nonorthogonal double foliation. It proves the compatibility of Horndeski Lagrangians with observations in an effective field theory approach. New solutions with intriguing logarithmic singularities and asymptotically nonflat behavior are derived, evading previous uniqueness theorems.
Article
Chemistry, Physical
Christopher J. N. Coveney, David P. P. Tew
Summary: We propose a scalable single-particle framework for treating electronic correlation in molecules and materials based on Green's function theory. By introducing the Goldstone self-energy, we derive a size-extensive Brillouin-Wigner perturbation theory from the single-particle Green's function. This new ground state correlation energy, named Quasi-Particle MP2 theory (QPMP2), avoids the characteristic divergences in strongly correlated systems present in second-order Moller-Plesset perturbation theory and Coupled Cluster Singles and Doubles methods, and demonstrates excellent performance in reproducing exact ground state energy and properties of the Hubbard dimer as well as larger Hubbard models.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Optics
D. E. Maison, L. Skripnikov
Summary: The francium atom is considered a potential candidate system to search for the T, P-violating electron electric dipole moment. Researchers demonstrate that the same experiment can also be used for the search of axionlike particles (ALP). By calculating the electronic structure constants of ALP-mediated interaction across a wide range of ALP masses, they show that the considered interactions, corresponding to the recently updated constraints on ALP-electron and ALP-nucleon coupling constants, can significantly contribute to the atomic electric dipole moment. Therefore, obtaining stronger restrictions on ALP characteristics in the francium atom electric dipole moment experiment is possible.
Article
Chemistry, Physical
Tobias Schafer, Florian Libisch, Georg Kresse, Andreas Gruneis
Summary: An embedding approach is presented to efficiently handle local electron correlation effects in periodic environments by integrating high-level correlation calculations into low-level ones. The method demonstrates accelerated convergence with respect to the local fragment size and has shown capabilities in accurately calculating adsorption energies of molecules and lattice impurities in solids.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Thomas M. Henderson, Ireneusz W. Bulik, Gustavo E. Scuseria
JOURNAL OF CHEMICAL PHYSICS
(2015)
Article
Chemistry, Physical
Alejandro J. Garza, Ireneusz W. Bulik, Thomas M. Henderson, Gustavo E. Scuseria
JOURNAL OF CHEMICAL PHYSICS
(2015)
Article
Chemistry, Physical
Alejandro J. Garza, IreneuszW. Bulik, Ana G. Sousa Alencar, Jianwei Sun, John P. Perdew, Gustavo E. Scuseria
Article
Chemistry, Physical
Alejandro J. Garza, Ireneusz W. Bulik, Thomas M. Henderson, Gustavo E. Scuseria
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2015)
Article
Physics, Multidisciplinary
J. P. F. LeBlanc, Andrey E. Antipov, Federico Becca, Ireneusz W. Bulik, Garnet Kin-Lic Chan, Chia-Min Chung, Youjin Deng, Michel Ferrero, Thomas M. Henderson, Carlos A. Jimenez-Hoyos, E. Kozik, Xuan-Wen Liu, Andrew J. Millis, N. V. Prokof'ev, Mingpu Qin, Gustavo E. Scuseria, Hao Shi, B. V. Svistunov, Luca F. Tocchio, I. S. Tupitsyn, Steven R. White, Shiwei Zhang, Bo-Xiao Zheng, Zhenyue Zhu, Emanuel Gull
Article
Chemistry, Physical
DeCarlos E. Taylor, Janos G. Angyan, Giulia Galli, Cui Zhang, Francois Gygi, Kimihiko Hirao, Jong Won Song, Kar Rahul, O. Anatole von Lilienfeld, Rafat Podeszwa, Ireneusz W. Bulik, Thomas M. Henderson, Gustavo E. Scuseria, Julien Toulouse, Roberto Peverati, Donald G. Truhlar, Krzysztof Szalewicz
JOURNAL OF CHEMICAL PHYSICS
(2016)
Article
Chemistry, Physical
Ireneusz W. Bulik, Michael J. Frisch, Patrick H. Vaccaro
JOURNAL OF CHEMICAL PHYSICS
(2017)
Article
Chemistry, Physical
Ireneusz W. Bulik, Michael J. Frisch, Patrick H. Vaccaro
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2018)
Article
Chemistry, Physical
Yao Cui, Ireneusz W. Bulik, Carlos A. Jimenez-Hoyos, Thomas M. Henderson, Gustavo E. Scuseria
JOURNAL OF CHEMICAL PHYSICS
(2013)
Article
Chemistry, Physical
Thomas M. Henderson, Ireneusz W. Bulik, Tamar Stein, Gustavo E. Scuseria
JOURNAL OF CHEMICAL PHYSICS
(2014)
Article
Chemistry, Physical
Ireneusz W. Bulik, Weibing Chen, Gustavo E. Scuseria
JOURNAL OF CHEMICAL PHYSICS
(2014)
Article
Chemistry, Multidisciplinary
Ireneusz W. Bulik, Robert Zalesny, Wojciech Bartkowiak, Josep M. Luis, Bernard Kirtman, Gustavo E. Scuseria, Aggelos Avramopoulos, Heribert Reis, Manthos G. Papadopoulos
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2013)
Article
Materials Science, Multidisciplinary
Ireneusz W. Bulik, Gustavo E. Scuseria, Jorge Dukelsky
Article
Materials Science, Multidisciplinary
Jianmin Tao, Ireneusz W. Bulik, Gustavo E. Scuseria